Achieving both super toughness and flame retardancy in polylactic acid (PLA) materials hinges on resolving the interface compatibility issues between flame retardants, toughening agents, and PLA, as well as overcoming potential antagonisms between these components. Here, we present an approach employing hyperbranched structures to simultaneously enhance the toughness and flame retardancy of PLA materials. Our strategy involved the reactive blending of PLA with a quaternary bio-based phosphorus-containing copolyester (PPE) featuring side hydroxyl groups and hexamethylene glycidyl cyclotriphosphazene (HGCP). The multi-epoxy groups of HGCP reacted with the hydroxyl and carboxyl groups present in PPE and PLA, resulting in the formation of hyperbranched PLA-PPE copolymers. The hyperbranched copolymers provided great interfacial compatibilization and low viscosity, synergistically promoting the melt-dripping flame-retardant mechanism facilitated by PPE, aiding in the rapid removal of heat and combustible material from the pyrolysis zone. Consequently, the PLA/PPE/HGCP blends exhibited super toughness, achieving a maximum notched impact strength of 70.2 kJ/m2. Additionally, the blends demonstrated a 27 % LOI and can pass the UL-94 V-0 rating. Moreover, all the blends are biodegradable in a Proteinase K solution. This research underscores the efficacy of utilizing hyperbranched structures as a promising strategy for the development of PLA materials with simultaneous enhancement of processability, toughness, and flame retardancy.
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