Poly(lactic acid) or poly(lactide) (PLA) is a renewable, bio-based, and biodegradable aliphatic thermoplastic polyester that is considered a promising alternative to petrochemical-derived polymers in a wide range of commodity and engineering applications. However, PLA is inherently brittle, with less than 10% elongation at break and a relatively poor impact strength, which limit its use in some specific areas. Therefore, enhancing the toughness of PLA has been widely explored in academic and industrial fields over the last two decades. This work aims to summarize and organize the current development in super tough PLA fabricated via polymer blending. The miscibility and compatibility of PLA-based blends, and the methods and approaches for compatibilized PLA blends are briefly discussed. Recent advances in PLA modified with various polymers for improving the toughness of PLA are also summarized and elucidated systematically in this review. Various polymers used in toughening PLA are discussed and organized: elastomers, such as petroleum-based traditional polyurethanes (PUs), bio-based elastomers, and biodegradable polyester elastomers; glycidyl ester compatibilizers and their copolymers/elastomers, such as poly(ethylene-co-glycidyl methacrylate) (EGMA), poly(ethylene-n-butylene-acrylate-co-glycidyl methacrylate) (EBA-GMA); rubber; petroleum-based traditional plastics, such as PE and PP; and various biodegradable polymers, such as poly(butylene adipate-co-terephthalate) (PBAT), polycaprolactone (PCL), poly(butylene succinate) (PBS), and natural macromolecules, especially starch. The high tensile toughness and high impact strength of PLA-based blends are briefly outlined, while the super tough PLA-based blends with impact strength exceeding 50 kJ m⁻² are elucidated in detail. The toughening strategies and approaches of PLA based super tough blends are summarized and analyzed. The relationship of the properties of PLA-based blends and their morphological parameters, including particle size, interparticle distance, and phase morphologies, are presented.

In this study, poly(lactic acid) (PLA)/starch blends were prepared through reactive melt blending by using PLA and starch as raw materials and vegetable oil polyols, polyethylene glycol (PEG), and citric acid (CA) as additives. The effects of CA and PEG on the toughness of PLA/starch blends were analyzed using a mechanical performance test, scanning electron microscope analysis, differential scanning calorimetry, Fourier-transform infrared spectroscopy, X-ray diffraction, rheological analysis, and hydrophilicity test. Results showed that the elongation at break and impact strength of the PLA/premixed starch (PSt)/PEG/CA blend were 140.51% and 3.56 kJ·m⁻², which were 13.4 and 1.8 times higher than those of pure PLA, respectively. The essence of the improvement in the toughness of the PLA/PSt/PEG/CA blend was the esterification reaction among CA, PEG, and starch. During the melt-blending process, the CA with abundant carboxyl groups reacted in the amorphous region of the starch. The shape and crystal form of the starch did not change, but the surface activity of the starch improved and consequently increased the adhesion between starch and PLA. As a plasticizer for PLA and starch, PEG effectively enhanced the mobility of the molecular chains. After PEG was dispersed, it participated in the esterification reaction of CA and starch at the interface and formed a branched/crosslinked copolymer that was embedded in the interface of PLA and starch. This copolymer further improved the compatibility of the PLA/starch blends. PEGs with small molecules and CA were used as compatibilizers to reduce the effect on PLA biodegradability. The esterification reaction on the starch surface improved the compatibilization and toughness of the PLA/starch blend materials and broadens their application prospects in the fields of medicine and high-fill packaging.

Ground tire rubber (GTR) with crosslinked structure shows hardly any plasticity and processability, giving rise to its relatively poor properties. The thermal-mechanical shearing devulcanization can effectively break the three-dimension crosslinked network structure and restore a certain extent of plasticity and processability. In this work, reclaimed rubber (RR) was obtained by thermal-mechanical shearing devulcanization as a potential filler for natural rubber. The vulcanization process, mechanical properties, microstructure of RR/natural rubber (NR) compounds composites were investigated. It was found that the NR vulcanizates containing 30 phr of RR as filler showed the higher tensile strength and elongation at break. Microstructural characterization analysis on a sample containing 30 phr of RR revealed the existence of strong interactions between the natural rubber matrix and RR, suggesting that RR and NR appeared to be well-matched, undergoing simultaneous curing and forming a continuous phase.