Direct milling: Efficient, facile, and green method for processing fibrillated cellulose/polymeric nanocomposites with boosted thermomechanical and rheological performance

Bringing biobased nanomaterials into polymer manufacturing is essential to enhance polymers' properties and address the challenges posed by plastic waste. Using polymers such as polyamide 6 (PA6) in advanced industries, e.g., automotive sector, has been impeded as a direct consequence of their inability to meet the required mechanical properties. Herein, we utilize bio-based cellulose nanofibers (CNFs) to enhance the properties of PA6 by green processing, with no footprint on the environment. We address the issue of the dispersion of the nanofillers in polymeric matrices and demonstrate direct milling (cryo-milling and planetary ball milling) to facilitate a thorough integration of the components. Nanocomposites incorporating 1.0 wt% CNF, processed by pre-milling followed by compression molding, are shown to possess a storage modulus of 3.8 ± 0.2 GPa, Young's modulus of 2.9 ± 0.2 GPa, and ultimate tensile strength of 63 ± 3 MPa (all measured at room temperature). To show the superiority of direct milling in achieving these properties, other frequent approaches used to disperse CNF in polymers, such as solvent casting and hand mixing, are meticulously investigated and compared for the performance of their resulting specimens. The ball-milling method is demonstrated to provide PA6-CNF nanocomposites with excellent performance, better than solvent casting, with no associated environmental concerns.