In-situ polycondensate-coated cellulose nanofiber heterostructure for polylactic acid-based composites with superior mechanical and thermal properties

Renewable yet biodegradable natural fiber (e.g., cellulose nanofiber (CNF)) reinforced bio-based polymers (e.g., polylactic acid (PLA)) are being applied for the manufacture of clean packaging products. The interface incompatibility between hydrophilic CNF and hydrophobic PLA still restricts the promotion of high-performance bio-based products. Herein, a polycondensate-coated CNF hybrid, wherein silane, aluminate, and titanate coupling agent monomers were in-situ polymerized onto the CNF surface via dehydration self-condensation, was designed and further employed as strengthening/toughening nanofillers for fabricating the CNF-reinforced PLA composite. Results showed that the polycondensate coatings could efficiently promote the dispersion of CNFs and enhance interfacial compatibility between CNFs and PLA. Attributing to the synergistic effect of polycondensate coatings and CNFs, a considerable improvement in processing, mechanical and thermal properties was obtained in resultant CNF/PLA composites. With adding 2.5 wt% polycondensate-coated CNFs, the tensile strength, Young's modulus, and tensile toughness of CNF-reinforced PLA composites was raised by about 27 %, 51 % and 68 %, respectively; also, such composite possessed greater elasticity and higher melt strength than pure PLA. This study provides a novel interface control strategy to fabricate low-cost yet high-performance PLA-based composites for sustainable packaging application.