Biomimetic adhesive containing nanocomposite hydrogel with enhanced materials properties

Chemically crosslinked polyacrylamide (PAAm) nanocomposite hydrogels were prepared with inorganic nano-silicate, Laponite, and dopamine methacrylamide (DMA). DMA consists of a biomimetic adhesive side chain covalently linked to a polymerizable methacrylate monomer. Copolymerizing DMA into a PAAm hydrogel strongly enhanced the interfacial interaction between the polymer network and Laponite. Nanocomposite hydrogels demonstrated reduced water content and increased materials properties that were dependent on both the Laponite and DMA contents. While increasing Laponite content alone improved materials properties moderately, these improvements were drastically enhanced when DMA is incorporated as measured by both unconfined compression testing and oscillatory rheometry. DMA-containing nanocomposite hydrogels demonstrated increased stiffness as well as excellent energy dissipation capability. Nanocomposite hydrogels with relatively low DMA and Laponite contents (2 to 3 wt% for each) demonstrated maximum compressive stress, elastic modulus, toughness, and storage and loss moduli values that were over an order of magnitude higher than control gels. DMA-containing nanocomposite hydrogels also demonstrated improved fracture resistance to compressive loading, capable of repeated compressed to 80% strain without rest for over 10 times while exhibiting compressive stress of over 1.1 MPa. The catechol side chain of DMA likely formed strong physical bonds with Laponite, which can dissipate fracture energy while minimizing permanent damage to the network architecture.