Constructing synergistically strengthening-toughening 3D network bundle structures by stereocomplex crystals for manufacturing high-performance thermoplastic polyurethane nanofibers reinforced poly(lactic acid) composites

As one of the most promising biodegradable materials, poly(lactic acid) (PLA) is seriously restricted by its notorious inherent brittleness and weak heat distortion resistance. In this work, a novel and simple methodology is proposed using an eccentric rotor extruder (ERE) with a predominantly elongational flow field to manufacture high-performance engineered poly(L-lactic acid)/poly(D-lactic acid)/thermoplastic polyurethane nanofiber composites on an industrial scale. The oriented tough TPU nanofibers (TNFs), rigid integrated PLA hybrid crystals and their good interface compatibility produce a strengthening-toughening bundle structure. When the PDLA content reached 3 wt%, the bundle structures interlinked with each other to form a strengthening-toughening 3D network. This resulted in a high-performance engineered 80L/5D/15T nanofiber composite with super toughness of 74.1 kJ/m2, high strength of 47.3 MPa and superior Young's modulus of 1378 MPa, which are 28.6 times, 85% and 92.7%, respectively, compared with neat PLLA. Compared with those published literatures, the 80L/5D/15T nanofiber composite not only possesses super toughness (more than 28 times) but also maintains good strength (maintain 85%), additionally good heat distortion resistance was also obtained. The performance of 80L/5D/15T nanofiber composite was significantly superior in comparison with biodegradable plastics as well as petroleum-based non-degradable general-purpose plastics and engineering plastics, demonstrating its enormous potential as a substitute structural material in harsh environments. It is believed that the novel and industrial scale methodology opens new perspectives for manufacturing other high-performance engineered biodegradable materials.