Unprecedented access to strong and ductile poly(lactic acid) by introducing In Situ Nanofibrillar Poly(butylene succinate) for green packaging.

The notion of toughening poly(lactic acid) (PLA) by adding flexible biopolymers has generated enormous interest but has yielded few desirable advances, mainly blocked by the sacrifice of strength and stiffness due to uncontrollable phase morphology and poor interfacial interactions. Here the phase control methodology, that is, intense extrusion compounding followed by "slit die extrusion-hot stretching-quenching" technique, was proposed to construct well-aligned, stiff poly(butylene succinate) (PBS) nanofibrils in the PLA matrix for the first time. We show that generating nanosized discrete droplets of PBS phase during extrusion compounding is key to enable the development of in situ nanofibrillar PBS assisted by the shearing/stretching field. The size of PBS nanofibrils strongly dependent on the PBS content, showing an increased average diameter from 83 to 116 and 236 nm for the composites containing 10, 20, and 40 wt % nanofibrils, respectively. More importantly, hybrid shish-kebab superstructure anchoring ordered PLA kebabs were induced by the PBS nanofibrils serving as the central shish, conferring the creation of tenacious interfacial crystalline ligaments. The exceptional combination of strength, modulus, and ductility for the composites loaded 40 wt % PBS nanofibrils were demonstrated, outperforming pure PLA with the increments of 31, 51, and 72% in strength, modulus, and elongation at break (56.4 MPa, 1702 MPa, and 92.4%), respectively. The high strength, modulus, and ductility are unprecedented for PLA and are in great potential need for packaging applications.