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Due to the increasing demand for modified polylactide (PLA) meeting “double green” criteria, the research on sustainable plasticizers for PLA has attracted broad attentions. This study reported an open-ring polymerization method to fabricate cellulose (MCC)-g-PCL (poly (ε-caprolactone)) copolymers with a fully sustainable and biodegradable component. MCC-g-PCL copolymers were synthesized, characterized, and used as green plasticizers for the PLA toughening. The results indicated that the MCC-g-PCL derivatives play an important role in the compatibility, crystallization, and toughening of the PLA/MCC-g-PCL composites. The mechanical properties of the fully bio-based PLA/MCC-g-PCL composites were optimized by adding 15 wt% MCC-g-PCL, that is, the elongation at break was 22.6% (~376% higher than that of neat PLA), the tensile strength was 47.3 MPa (comparable to that of neat PLA), and the impact strength was 26 J/m (~130% higher than that of neat PLA). DSC results indicated that MCC-g-PCL reduced the T g  of the PLA blend. When the addition amount was 15 wt%, the T g  of the blend was 58.4°C. Compared with MCC, MCC-g-PCL polyester plasticizer has better thermal stability, T 5%  (°C) can still be maintained above 300°C. The rheological results showed that MCC-g-PCL acted as a plasticizer, the introduction of PCL flexible chain increased the mobility of PLA molecular chain, and decreased the complex viscosity, storage modulus and loss modulus of PLA blends. The MCC-g-PCL derivatives, as a new green plastic additive, have shown an interesting prospect to prepare fully bio-based composites.

Fully Bio-Based Composites of Poly (Lactic Acid) Reinforced with Cellulose-Graft-Poly-(ε-Caprolactone) Copolymers