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Constructing stereocomplex (SC) crystallites at the interface of poly(L‐lactide) (PLLA)/elastomer blends represent a promising strategy to develop heat‐resistant and super‐tough PLLA materials because such SC crystallites can behave as not only nucleator to accelerate crystallization of PLLA matrix but also interfacial binder to strengthen interface. The properties of blends could be largely dominated by the SC interfacial layer, however, it is still unclear how the interfacial structure affects nucleating efficiency and interfacial strength. Herein, taking PLLA/poly(ethylene‐co‐methyl acrylate‐graft‐poly(D‐lactide)) (EMA‐g‐PDLA) blends as an example, EMA‐g‐PDLA bearing different chain lengths and grafting densities is prepared to tailor the size and packing density of interface‐localized SC crystallites. The results indicate that the interfacial structure and properties of the blends have been successfully manipulated. Compared with low‐graft‐density long PDLA chains, high‐graft‐density short ones can readily collaborate with PLLA chains to form numerous SC crystallites with smaller size and higher packing density at the interface and thus dramatically enhance the impact toughness and matrix crystallization rate. Moreover, the toughness is dominated by the content of SC crystallites, but the matrix crystallization is determined by their size and packing density. The work provides a new understanding of SC structure controlling the properties of PLLA/elastomer blends. [ABSTRACT FROM AUTHOR]

In recent years, rubber toughened polypropylene (PP) blends have been extensively investigated with special regard to the importance of PP matrix properties (e.g., crystal morphology and structure) in tailoring the toughening efficiency. Unfortunately, although high melt flowability is indispensable to the processing of polymers into complex thin-wall products, it remains a huge challenge to achieve a marvelous balance between stiffness and toughness in the blends with relatively low matrix molecular weight. Herein, taking PP/EPR (ethylene-propylene copolymer) blends as an example, the combined effects of matrix molecular weight and crystallinity on the mechanical properties of PP/EPR blends have been examined in both experiment and theory. The experimental results show that decreasing molecular weight leads to significant deterioration in notched impact toughness, tensile strength and Young's modulus. Impressively, the toughness loss caused by the decrease of molecular weight can be well-compensated by a slight reduction in the matrix crystallinity, without evidently sacrificing the strength and modulus, demonstrating an improved stiffness-toughness balance. Theoretical analysis indicates that the impact toughness of PP/EPR blends is heavily dependent on the chain entanglement density (v e) of PP matrix, and a linear relationship between critical interparticle distance (ID c) and the v e 1/3 has been verified from both experiment and theory. Moreover, it is interesting to find that decreasing matrix crystallinity can increase the v e of low-molecular-weight PP matrix, which enables the effective toughening at lower concentration of EPR and thus gives rise to less loss in the strength and modulus. We believe this work not only gives a new insight into the role of chain entanglement in the toughening but also provides a promising guidance for the design of high-performance PP with high melt flowability. [Display omitted] • Combined effects of M n and crystallinity on the toughening efficiency of PP/EPR blends were studded. • The relationship between the ID c and v e of PP matrix i.e. ID c ∼ v e 1/3 , was given for the first time. • Matrix with higher M n or lower crystallinity has higher v e , exhibiting larger ID c. • Toughness loss caused by decreasing M n can be compensated by reducing crystallinity. • Low-viscosity PP/EPR blends with good toughness-stiffness balance were obtained. [ABSTRACT FROM AUTHOR]

In this work, we report that super-toughened and high-strength polylactide/poly(butylene adipate-co-terephthalate) (PLA/PBAT) blends can be successfully prepared by interfacial compatibilization and dynamic vulcanization during reactive melt-blending with small amounts (0.5–3 wt %) of epoxy-functional styrene-acrylic oligomers (ESA). The results show that the compatibilization is realized with the grafting of some PLA and PBAT chains onto ESA backbones to in-situ generate PLA- graft -PBAT copolymers at the blend interface. Meanwhile, the ESA-mediated vulcanization gives rise to the highly cross-linked PBAT particles with a unique network-like distribution in the PLA matrix. Both the strengthened interfaces and networked PBAT particles are favorable to the triggering of massive matrix plastic deformation required for effective energy dissipation and thus the toughening effect is substantially enhanced. Impressively, the notched Izod impact toughness and elongation at break of the PLA/PBAT (70/30) blends can reach as high as 62.4 kJ/m2 and 232%, while the tensile strength increases from 44.2 MPa to 51.5 MPa, indicating a balanced toughness and strength. Most notably, it is demonstrated that tuning the molecular structure of ESA (i.e., epoxy group density and backbone length) is essential to improving the interfacial adhesion and phase morphology, enabling high toughening efficiency. Our facile yet robust strategy presents an unprecedented opportunity for the development of high-performance fully biodegradable PLA blends. [Display omitted] • Full biodegradable PLA/PBAT blends with balanced toughness and strength are prepared. • Dynamic vulcanization leads to the highly cross-linked PBAT domains in PLA matrix. • Copolymers are in-situ generated at the interface for effective compatibilization. • The formation of PBAT particle network is responsible for the desired properties. • The key role of ESA structure in tailoring the morphology and properties is verified. [ABSTRACT FROM AUTHOR]