Shape memory properties of two thermoplastic multiblock copolymers composed of poly(lactic acid) (PLA) and poly(ethylene glycol) (PEG) having different PEG‐segment lengths of 6 and 11 kDa were studied. The performance as a shape memory polymer at high strain level (600%) and its interrelations with shape‐programming conditions, molecular orientation, and microstructural changes are elucidated. A significant contribution of strain‐induced crystallization of PLA segments to the improvement of temporary shape fixation was evidenced upon increasing draw ratio and/or shape‐holding duration as well as programming temperature (within certain range) without largely sacrificing the shape recoverability. Series of microstructural characterizations reveal the occurrence of fibrillar‐to‐lamellar transformation upon shape recovery (at 60 °C) of the samples programmed at 40 °C, generating shish–kebab crystalline morphology. Such phenomenon is responsible for the high‐strain shape memory effect of these materials. The unprecedented formation of shish–kebab structure at such relatively low temperature (instead of the melting temperature range) in solid state observed in these copolymers as well as their high‐strain shape memory functionality would bestow the promising future for their practicability in diverse areas. © 2018 Wiley Periodicals, Inc. J. Polym. Sci., Part B: Polym. Phys. 2019, 57, 241–256

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The frozen instant food packaging is the one of disposal product, which produced from petroleum–based plastic and has been accumulated worldwide pressuring on the environment. Therefore, the biodegradable plastics have become key candidates in this application. Poly(lactic acid) (PLA) was regarded as one of the most promising biodegradable polymer due to its good mechanical properties. The aim of this work was to study on the freezability and microwavability of PLA through crosslink reaction. For the improvement of the processibility of PLA, hyperbranched polymer (HBP) and polypropylene glycol (PPG) were used as plasticizer. Then the crosslinking of PLA was introduced by addition of peroxide (Luperox101) and triallyl isocyanurate (TAIC) in an internal mixer. Neat and modified PLA samples were characterized and testing for mechanical properties. From the gel content results, it was showed the increased value with the increased content of TAIC due to the denser crosslinked structure of polymer. This result was confirmed by FT-IR spectra. All modified PLA samples showed the higher %strain at break than neat PLA. In addition, impact resistance in frozen state showed the results of modified PLA with 0.1wt% of peroxide and 0.15 wt% of TAIC, was higher than neat PLA. Moreover, this composition also showed the highest microwave response and heat accumulation was suppressed when the specimen was immersed in the water during the test. From the results obtained in this work, the further investigation is needed to pursue and elucidate the relationship between the polymer structure and heat absorption when materials undergo the microwave radiation.