Cellulose nanofibrils as reinforcing agents for PLA-based nanocomposites: An in situ approach

One-pot in situ polymerization approach was explored for the preparation of polylactide (PLA)-cellulose nano-fibril (CNF) bio-nanocomposites. CNF were first prepared through enzymatic and mechanical treatment of bleached hardwood kraft pulp. The bio-nanocomposites- were then fabricated through ring opening polymerization (ROP) of L-lactide, in the presence of various amounts of fibrils. Molecular weight, thermal properties, surface morphology, mechanical and wettability properties of the PLA-CNF nanocomposites were evaluated. DSC analysis demonstrated the effect of CNF on crystallization and crystalline morphology of PLA. Improved modulus for the nanocomposites with respect to standard PLA was demonstrated, however, the differences in tensile stress were small probably due to the counteracting effects of reinforcement from CNF and the decreasing molecular weight as a function of CNF concentration. The absence of pulled-out fibers was assessed, highlighting the strong interface and covalent attachment of PLA chains on CNF surface. Finally, the covalent bonding of PLA chains on CNF surface was demonstrated by isolating the non-soluble part, consisting of PLA-grafted CNF, and characterization of this residue.