High-Performance Polylactide Vitrimers via Polyol-Assisted Network Engineering through Reactive Blending

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Abstract Polylactide (PLA) is a promising biobased and biodegradable polymer, but its limited heat resistance and mechanical performance hinder broader engineering applications. Herein, high-strength and reprocessable PLA vitrimers were prepared through a facile reactive blending strategy. A multifunctional polyol, bis(2-hydroxyethyl)imino-tris(hydroxymethyl)methane (BTM), was incorporated into PLA chains via internal-catalyzed transesterification, followed by cross-linking with 4,4′-methylenediphenyl diisocyanate (MDI) to form a dynamic covalent network. The resulting PLA vitrimers exhibited enhanced mechanical strength, toughness, thermal stability, and water resistance while retaining reprocessability. The optimal sample achieved a tensile strength of 93.4 MPa (42% higher than neat PLA) without compromising ductility, and retained its shape at 120 °C. Furthermore, a biobased long-chain polyol (GTA) was employed to tailor the network architecture, leading to a more balanced combination of strength and toughness. This work demonstrates an effective strategy for transforming commercial PLA into high-performance, recyclable materials for sustainable engineering plastics.

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