Constructing Bone-Mimicking High-Performance Structured Poly(lactic acid) by an Elongational Flow Field and Facile Annealing Process

Poly(lactic acid) (PLA) as one of the most promising biodegradable polymers is being tremendously restricted in large-scale applications by the notorious toughness, ductility, and heat distortion resistance. Manufacturing PLA with excellent toughness, considerable ductility, balanced strength, and great heat distortion resistance simultaneously is still a great challenge. Natural structural materials usually possess excellent strength and toughness by elaborately constructed sophisticated hierarchical architectures, however, completely reproducing natural structural materials' architecture have evidenced to be difficult. Inspired by the hierarchical construction of the compact bone, an innovational method with an intensive and continuous elongational flow field and facile annealing process was developed to create bone-mimicking structured PLA at an industrial scale. The bone-mimicking structured PLA with unique and novel hierarchical architectures of interlocked 3D network lamellae and large extended-chain lamellae connecting the regular lamellae was constructed by in situ formed oriented thermoplastic poly(ether)urethane nanofibers (TNFs) acting as "collagen fibers", orderly staggered PLA lamellae behaving as "hydroxyapatite (HA) nanocrystals", and the tenacious interface functioning as a "soft protein" adhesive layer. Attributed to the unique structure, it possesses super toughness (90.3 KJ/m2), high stiffness (2.15 GPa), balanced strength (52.6 MPa), and notable heat distortion resistance (holding at 163 °C for 1 h) simultaneously. These excellent performances of the structured PLA provide it with immense potential applications in both structural and bio-engineering materials fields such as artificial bones and tissue scaffolds.