Fused Deposition Modeling of Isotactic Polypropylene/Graphene Nanoplatelets Composites: Achieving Enhanced Thermal Conductivity Through Filler Orientation

High-performance thermally conductive composites are increasingly vital due to the accelerated advancements in communication and electronics, driving the demand for efficient thermal management in electronic packaging, light-emitting diodes (LEDs), and energy storage applications. Controlling the orderly arrangement of fillers within a polymer matrix is acknowledged as an essential strategy for developing thermal conductive composites. In this study, isotactic polypropylene/GNP (iPP/GNP) composite filament tailored for fused deposition modeling (FDM) was achieved by combining ball milling with melt extrusion processing. The rheological properties of the composites were thoroughly studied. The shear field and pressure field distributions during the FDM extrusion process were simulated and examined using Polyflow, focusing on the influence of the 3D printing processing flow field on the orientation of GNP within the iPP matrix. Exploiting the unique capabilities of FDM and through strategic printing path design, thermally conductive composites with GNPs oriented in the through-plane direction were 3D printed. At a GNP content of 5 wt%, the as-printed sample demonstrated a thermal conductivity of 0.64 W/m · K, which was 1.5 times the in-plane thermal conductivity for 0.42 W/m · K and triple pure iPP for 0.22 W/m · K. Effective medium theory (EMT) model fitting results indicated a significantly reduced interface thermal resistance in the through-plane direction compared to the in-plane direction. This work shed brilliant light on developing PP-based thermal conductive composites with arbitrarily-customized structures.