Tailoring Crystalline Morphology by High-Efficiency Nucleating Fiber: Toward High-Performance Poly(l-lactide) Biocomposites

In this work, a high-melting-point poly(l-lactide) fiber (hPLLA fiber) with high-efficiency nucleation activity was prepared and introduced into PLLA matrix to prepare fully biodegradable PLLA biocomposites. The highly active nucleating surfaces of the hPLLA fiber induced chain ordering and lamellar organization, leading to a preferable formation of well-organized PLLA transcrystallinity at the surface of the hPLLA fiber under quiescent conditions. The construction of such compact transcrystallinity increased the crystallinity and enhanced the interfacial adhesion, which largely promoted heat resistance, tensile strength, and barrier property of PLLA biocomposites at a low content of hPLLA fiber. With the addition of 1 wt % hPLLA fiber, the storage modulus of the PLLA biocomposite was enhanced by 82 times from 4 to 330 MPa at 80 °C and the oxygen permeability coefficient and water permeability coefficient were decreased by 52 and 51% to be 5.9 × 10–15 cm3·cm/cm2·s·Pa and 4.5 × 10–14 g·cm/cm2·s·Pa, respectively, compared with those of pure PLLA. Moreover, the transparency of PLLA was maintained with the incorporation of hPLLA fiber. Thus, this strategy paved a new way to prepare high-performance and fully biodegradable biocomposites.