Selectively multilayered distribution of stereocomplex crystallite and poly(3-hydroxybutyrate-co-3-hydroxyvalerate) ribbons to achieve highly ductile and strong poly(l-lactide) composites

Abstract

Blending poly(l-lactide) (PLLA) with elastic polymers is an efficient way to obtain highly ductile materials (> 300 %), but it is accompanied by a significant reduction in strength. In this work, a special alternating multilayered composites with alternating stereocomplex crystallite (SC) (PLLA/poly(d-lactide) (PDLA) layer) and highly oriented Poly(3-hydroxybutyrate-co-3-hydroxyvalerate) (PHBV) ribbons (PLLA/PHBV layer) is in situ constructed during laminated structuring process. Experimental results show that in situ formed PHBV ribbons are limitedly distributed in the thickness direction and align parallel to the layer interfaces. More interestingly, not only highly oriented shish crystals but also sparse lamellae of PLLA, which are arrested by SC, shish crystals, and PHBV ribbons, are in situ formed. Compared with sea−island structured composites prepared by traditional compression molding, the alternating multilayered composites show an increase in elongation at break from 8.7 % to 345.1 % and an increase in yield strength from 61.4 MPa to 73.2 MPa. During the tensile testing, the PLLA/PHBV layers firstly form micro-fibrils and micro-voids, driving the molecular chains of the PLLA/PDLA layer to respond in time to external forces through stress transfer of rich continuous layer interfaces. Since shear yielding and plastic deformation can easily penetrate the entire matrix, the alternating multilayered composites go a brittle-ductile transformation and the ductility is improved significantly. The increased strength of the alternating multilayered material is ascribed to the stiff shish crystals and SC. This work provides important guidance for the durable application of strong and ductile PLLA-based materials.