3D printed lignin/polymer composite with enhanced mechanical and anti-thermal-aging performance

Lignin is the most abundant natural aromatic polymer globally but is still underutilized as a renewable material, even with its versatile properties. One approach to using lignin is to incorporate it in polymer composites, but this application is often limited by the poor mechanical performance of the resultant composite due to the poor interfacial adhesion. Following the structure-property relationship, stronger interactions were designed to be enhanced by alternating the functional groups of lignin. This study applied a demethylation method to hardwood lignin (Ori-Lig) to introduce more phenolic hydroxyl groups. Research studies with rheology behavior and molecular simulations demonstrated that an increased phenolic hydroxyl content could improve the adhesion between the modified lignin (OH-Lig) and the polymer matrix at the interface. The tensile performance of the samples from the fused depositional modeling (FDM) 3D printing technique was also improved due to the improved interfacial adhesion. Specifically, by adding 10 wt% of the modified lignin, the tensile strength of the 3D printed samples could reach 46.1 MPa (40.2 MPa of Polyamide 12, PA12), and Young's Modulus could be improved to 1.73 GPa (1.48 GPa of PA12). OH-Lig also improved anti-aging performance so that the tensile strength of the OH-Lig composite after thermo-aging (100 h at 140 degrees C) remained similar to 48 MPa. The enhanced mechanical performance with anti-aging properties indicated that the OH-Lig composite may replace PA12 to reduce the use of petrol-based materials. This work showed the method of purposefully designing and modifying lignin structures to fulfill the interaction requirements between lignin and polymer matrix. The as-prepared lignin could be used to prepare functional composites to achieve improved mechanical performance and targeted functions at the same time.