Development of 3D-Printing Filament from Recycled Low-Density Polyethylene (rLDPE) and High-Density Polyethylene (rHDPE) Composites Reinforced with Lignin Additive

This study investigates the development of sustainable composite materials using recycled low-density polyethylene (rLDPE) and high-density polyethylene (rHDPE) in an 80/20 mass ratio, incorporating kraft lignin as a bio-derived additive and polyethylene-graft-maleic anhydride (PE-g-MA) as a compatibilizer. Reactive melt mixing was employed to produce composites with varying lignin loadings (1, 3, 5, and 10 wt%). The structural, thermal, and mechanical properties and segmental dynamics of the materials were thoroughly examined using differential scanning calorimetry (DSC), infrared spectroscopy (IR), X-ray photoelectron spectroscopy (XPS), X-ray diffraction (XRD), thermogravimetric analysis (TGA), pyrolysis-gas chromatography/mass spectrometry (Py-GC/MS), tensile testing, scanning electron microscopy (SEM), and dielectric relaxation spectroscopy (DRS). The incorporation of lignin exhibited minimal disruption to the polymeric thermal transitions, while it boosted thermal stability, as confirmed by the TGA curves. According to the segmental dynamics findings, the glass transition temperature of the polymeric blend (-35 °C) was increased systematically with the addition of lignin by ~1-20 K. Tensile tests showed that the 1 wt% additive ratio demonstrated the optimal balance of strength and ductility. Morphological observations supported these findings, revealing uniform dispersion at low additive ratio and increased agglomeration at higher ratios. Based on its superior performance, the composite containing 1 wt% lignin was successfully extruded into filament suitable for 3D-printing. This study highlights the synergy of bio-based additives and recycled polymers in engineering high-performance materials, promoting circular economy principles and reduced environmental footprint through upcycling post-consumer waste into functional, valuable products.