Four-Dimensional Printing of Auxetic Structures Using Nanocellulose-Reinforced PLA/PETG Blends

Abstract

This study explores the development of 4D-printed smart structures based on PLA/PETG (75/25) polymer blends reinforced with nanocellulose (0–3 wt%), processed using fused filament fabrication (FFF). Both conventional U-shaped specimens and anti-tri-chiral auxetic architectures were fabricated to evaluate the effects of nanocellulose on mechanical performance and shape memory behavior. Tensile tests demonstrated that nanocellulose reinforcement enhanced both strength and stiffness, with the highest values observed at 2 wt% (tensile strength of 56 MPa and Young’s modulus of 3.3 GPa). In standard U-shaped samples, all compositions showed excellent shape fixity and recovery (100%). For auxetic structures, shape memory behavior and deformation response varied with nanocellulose content. Notably, 2 wt% nanocellulose yielded the highest shape recovery ratio (90.8%) and fixity (99.8%), indicating improved elasticity and structural responsiveness. Meanwhile, 1 wt% nanocellulose resulted in the highest energy absorption and more controlled deformation under compression, suggesting enhanced energy dissipation and stress distribution. A slight decrease in performance at 3 wt% is attributed to nanocellulose agglomeration and reduced polymer chain mobility. These findings highlight nanocellulose as a multifunctional additive that enables fine-tuning of mechanical and functional properties in 4D-printed structures. Depending on the intended application whether focused on energy absorption, mechanical strength, or shape recovery nanocellulose content can be strategically adjusted. This approach opens pathways for designing responsive materials suited for biomedical engineering, adaptive devices, and advanced environmental technologies.