Polymer Network Editing of Elastomers for Robust Underwater Adhesion and Tough Bonding to Diverse Surfaces

Tough adhesives with robust adhesion are desperately needed for biomedical and technological applications. However, it is extremely challenging to engineer tough and durable adhesives that are simple to make yet also exhibit strong underwater adhesion as well as tough bonding to diverse surfaces. Here, we report bioinspired elastomers based on water-immiscible polydiolcitrates, where their tough mechanical properties, robust underwater adhesion (80 kPa), and tough bonding performance (with an interfacial toughness >1000 J m^–2 and a shear and tensile strength >0.5 MPa) to diverse solid materials (glass, ceramics, and steel) are actuated by the incorporation of trace amounts of additives. The additives could edit the polymer networks during the elastomer polymerization by dramatically regulating the cross-linking structures of covalent and reversible bonds, the length of polymer chains, and the hydrophobic and hydrophilic motifs, which markedly tuned the mechanical and adhesive properties of the bioelastomers. We also demonstrate versatile applications of the durable elastomers, as tough flexible joints for solid materials, superglue, tissue sealants, hemostatic dressing, and wound repair.