Additively-Manufactured High-Concentration Nanocellulose Composites: Structure and Mechanical Properties

Additive manufacturing technology (AMT) has transformed polymer composites' manufacturing process with its exceptional ability to construct complex products with unique materials, functions, and structures. Besides limiting studies of manufacturing arbitrarily shaped composites using AMT, printed structures with a high concentration of nanocellulose face adhesion issues upon drying, resulting in shape fidelity issues and low mechanical strength. This research demonstrates an economical approach to printing a high-concentration (25.46 wt%) nanocellulose (NC) layer-wise pattern to fabricate structures. Two different composites are fabricated: (1) 3D-printed pure and high-concentration (10, 15, and 20 wt%) polyvinyl-alcohol (PVA)-blended NC structures followed by freeze-drying and impregnation of Epofix resin by varying hardener contents; (2) 3D-printed PVA-blended NC green composites dried at cleanroom conditions (Relative humidity 45%; Temperature 25 °C). Different contents (10, 15, and 20 wt%) of PVA as a crosslinker were blended with NC to assist the printed layers' adhesions. An optimum PVA content of 15 wt% and an Epofix resin with 4 wt% hardener cases showed the highest bending strength of 55.41 ± 3.63 MPa and elastic modulus of 4.25 ± 0.37 GPa. In contrast, the 15 wt% PVA-blended NC cleanroom-dried green composites without resin infusion showed bending strength and elastic modulus of 94.78 ± 3.18 MPa and 9.00 ± 0.27 GPa, reflecting high interface adhesions as confirmed by scanning electron microscope. This study demonstrated that AMT-based nanocellulose composites could be scaled up for commercial use.