This study investigates how the molecular architecture of functional tetracyclotetrasiloxane derivatives (CS) influences the mechanical and physicochemical properties of polylactide (PLA) under accelerated aging conditions (UV radiation at 313 nm, elevated temperature, and water mist), aiming at durable applications. Two novel tetracyclotetrasiloxane-derived modifiers, CS-MA-3HEX and CS-2MA-2HEX were synthesized to enhance PLA impact toughness.
Comprehensive, multifactorial analytical methods were employed to characterize the modifiers and their impact on PLA performance. Experimental results demonstrate that applied modifiers act as effective macromolecular plasticizers, significantly improving the initial ductility of PLA (ɛb ∼535% increase) and impact toughness (∼180%). However, the beneficial effects of the modification were not permanent. Aging resulted in significant embrittlement and mechanical deterioration of both PLA and PLA/CS samples, indicating limited long-term stability of the plasticized PLA, attributed to chain scission and increased crystallinity. Nevertheless, the Tg of PLA/CS remained stable during aging, indicating preserved thermal stability despite mechanical degradation. These findings underline that functionalized tetracyclosiloxanes enhance the initial mechanical performance of PLA and enable moderation of the degradation rate by adjusting the methacrylate group content in the modifier particle, supporting the design of materials with tunable service lifetimes for specific applications.
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