Fabrication of Tough and Heat‐Resistant Polylactic Acid ( PLA ) Melt‐Blown Nonwovens by In Situ Hybridization Fibrillation of Polyamide 11

ABSTRACT This work proposes an in situ hybrid fibrillation strategy to simultaneously enhance the toughness and thermal resistance of fully bio‐based polylactic acid (PLA) melt‐blown nonwovens (MBNs). A reactive PLA/(PA11/G‐HNTs) ternary gradient blending system was designed in which polyamide 11 (PA11) serves as a ductile fibrillating phase and epoxidized halloysite nanotubes (G‐HNTs) act as nanoscale skeletons of reinforcing agents. The tailored interfacial reactions and rheological tuning enable PA11 to undergo stable in situ microfibrillation during melt‐blown, while G‐HNTs align along the fibril axis to form a hierarchical “microfibril–nanotube” hybrid network. Structural analyses (SEM, TEM, DSC, DMA, rheology) reveal a clear transition from a droplet–matrix morphology to a fibril‐reinforced architecture, accompanied by improved crystallization and melt strength. The optimized PLA/(PA11/G‐HNTs) MBNs achieve more than a 150% increase in elongation‐at‐break, as well as exhibit 20°C–30°C higher dry‐heat dimensional stability compared with neat PLA MBNs. These findings demonstrate a scalable, melt‐processing‐compatible route for producing super‐tough and heat‐resistant PLA melt‐blown nonwovens.