Comparative study of blending techniques in polylactic acid/cellulose nanofibrils green composites for benchtop <scp>3D</scp> printing filaments

Abstract Additive manufacturing for polylactic acid (PLA) reinforced with cellulose nanofibrils (CNF) could unlock fabrication of specialized and user‐specific biomedical devices. However, the process of combining PLA and CNF is challenging and proves complicated with possible irreversible CNF agglomeration and organic solvents leftover, particularly when involving solvent‐casting technique. Direct melt‐blending can mitigate these issues, but there are few reports of a single‐step melting and extrusion process to produce ready‐to‐use 3D printing filaments. This study compares the distribution of CNF fillers within the PLA matrix in PLA/CNF composites made by direct melt‐blending into filaments using a benchtop filament maker, and by solvent‐casting followed by extrusion into filaments. The filaments were 3D‐printed via fused deposition modeling (FDM), followed by tensile testing, morphology, and other characterizations. Uneven filament diameters were observed for the composite filaments prepared via solvent‐casting because of severe agglomeration, resulted in poor printability and tensile properties of filaments and 3D‐printed samples. Direct melt‐blended filament diameters were consistent, resulted in only slight decrease of tensile properties compared to pure PLA, contributing to the highest maximum tensile strength of 3D‐printed sample of 51.47 ± 1.73 MPa at 5% CNF loading. Morphology revealed good integration of CNF into PLA matrix starting at 3% CNF loading. Direct melt‐blending was comparable to the conventional methods, which enables simpler PLA/CNF composite preparation especially for 3D printing. Highlights Better dispersibility achieved by direct melt‐blending than by solvent‐casting. PLA/CNF filaments produced via solvent‐casting suffered severe agglomeration. Direct melt‐blended PLA/CNF5% yielded the highest maximum tensile strength. Morphology reveals good CNF‐PLA integration starting at 3% of CNF loading. Worsened agglomeration causing increased number of voids observed at 10% CNF.