A supramolecular hydrogel leveraging hierarchical multi-strength hydrogen-bonds hinged strategy achieving a striking adhesive-mechanical balance

Abstract

To obtain high-performance tissue-adhesive hydrogel embodying excellent mechanical integrity, a supramolecular hydrogel patch is fabricated through in situ copolymerization of a liquid-liquid phase separation precursor composed of self-complementary 2-2-ureido-4-pyrimidone-based monomer and acrylic acid coupled with subsequent corporation of bioactive epigallocatechin gallate. Remarkably, the prepared supramolecular hydrogel leverages hierarchical multi-strength hydrogen-bonds hinged strategy assisted by alkyl-based hydrophobic pockets, broadening the distribution of binding strength of physical junctions, striking a canonical balance between superb mechanical performance and robust adhesive capacity. Ultimately, the fabricated supramolecular hydrogel patch stands out as a high stretchability (1500 %), an excellent tensile strength (2.6 MPa), a superhigh toughness (12.6 MJ m⁻³), an instant and robust tissue adhesion strength (263.2 kPa for porcine skin), the considerable endurance under cyclic loading and reversible adhesion, a superior burst pressure tolerance (108 kPa) to those of commercially-available tissue sealants, and outstanding anti-swelling behavior. The resultant supramolecular hydrogel patch demonstrates the rapid hemorrhage control within 60 s in liver injury and efficient wound closure and healing effects with alleviated inflammation and reduced scarring in full-thickness skin incision, confirming its medical translation as a promising self-rescue tissue-adhesive patch for hemorrhage prevention and sutureless wound closure.