Fully Biobased Shape Memory Thermoplastic Vulcanizates from Poly(Lactic Acid) and Modified Natural Gum with Co-Continuous Structure and Super Toughness.

Novel, fully biobased shape memory thermoplastic vulcanizates (TPVs) were prepared using two sustainable biopolymers, poly(lactic acid) (PLA), and modified natural gum (EUG--GMA), via a dynamic vulcanization technique. Simultaneously, in situ compatibilization was achieved in the TPVs to improve interfacial adhesion and the crosslinked modified gum (EUG) was in "netlike" continuous state in the PLA matrix to form "sea-sea" phase structure. The promoted interface and co-continuous structure played critical roles in enhancing shape memory capacity and toughness of the TPVs. The TPV with 40 wt % modified EUG displayed the highest toughness with an impact strength of 54.8 kJ/m and the most excellent shape memory performances with a shape fixity ratio () of 99.83% and a shape recovery ratio () of 93.74%. The prepared shape memory TPVs would open up great potential applications in biobased shape memory materials for smart medical devices.