Bio-Inspired Hydrogen-Bond Cross-Link Strategy toward Strong and Tough Polymeric Materials

It remains a huge challenge to create advanced polymeric materials combining high strength, great toughness, and biodegradability so far. Despite enhanced strength and stiffness, biomimetic materials and polymer nanocomposites suffer notably reduced extensibility and toughness when compared to polymer bulk. Silk displays superior strength and toughness via hydrogen bonds (H-bonds) assembly, while cuticles of mussels gain high hardness and toughness via metal complexation cross-linking. Here, we propose a H-bonds cross-linking strategy that can simultaneously strikingly enhance strength, modulus, toughness, and hardness relative to polymer bulk. The H-bond cross-linked poly­(vinyl alcohol) exhibits high yield strength (∼140 MPa), reduced modulus (∼22.5 GPa) in nanoindention tests, hardness (∼0.5 GPa), and great extensibility (∼40%). More importantly, there exist semiquantitive linear relationships between the number of effective H-bond and macroscale properties. This work suggests a promising methodology of designing advanced materials with exceptional mechanical by adding low amounts (≤1.0 wt %) of small molecules multiamines serving as H-bond cross-linkers.