Spider-silk inspired tough and self-healable lignin based hydrogel via synergistic hydrogen bonding for flexible...

Traditional hydrogels face challenges in flexible electronics due to their inherent mechanical weaknesses. Inspired by the strong yet flexible hierarchical structure of natural spider silk, this study developed an innovative "synergistic hydrogen-bond engineering" strategy to fabricate a bio-inspired hydrogel with high strength, high toughness, and self-healing ability. Without any chemical modification, we ingeniously incorporated renewable lignin (KL) and citric acid (CA) as synergistic reinforcing and crosslinking agents into a flexible poly(N,N-dimethylacrylamide) (PDMA) network. This design promotes the formation of lignin-rich phase-separated microdomains, which act as efficient dynamic physical crosslinks. These microdomains work together with a multi‑hydrogen-bond network to achieve remarkable energy dissipation. The resulting hydrogel achieves a tensile strength of 2.44 MPa and a fracture strain of 1237%, along with excellent repairability and remoldability. Benefiting from its inherent conductivity, the hydrogel exhibits a gauge factor of 3.40 within the 0-100% strain range and can reliably monitor diverse human motions, including finger, elbow, and knee bending. These attributes demonstrate its strong potential for developing durable and sensitive hydrogel-based strain sensors.