Improvement of the Thermal Conductivity and Mechanical Properties of 3D-Printed Polyurethane Composites by Incorporating Hydroxylated Boron Nitride Functional Fillers

Recently, the use of fused deposition modeling (FDM) in the three-dimensional (3D) printing of thermal interface materials (TIMs) has garnered increasing attention. Because fillers orient themselves along the direction of the melt flow during printing, this method could effectively enhance the thermal conductivity of existing composite materials. However, the poor compatibility and intensive aggregation of h-BN fillers in polymer composites are still detrimental to their practical application in thermally conductive materials. In this study, hydroxyl-functionalized boron nitride (OH-BN) particles were prepared by chemical modification and ultrasonic-assisted liquid-phase exfoliation to explore their impact on the surface compatibility, mechanical properties and the final anisotropic thermal conductivity of thermoplastic polyurethane (TPU) composites fabricated by FDM printing. The results show that the surface-functionalized OH-BN fillers are homogeneously dispersed in the TPU matrix via hydrogen bonding interactions, which improve the interfacial adhesion between the filler and matrix. For the same concentration of loaded filler, the OH-BN/TPU composites exhibit better mechanical properties and thermal conductivities than composites incorporating non-modified h-BN. These composites also show higher heat conduction along the stand-vertical direction, while simultaneously exhibiting a low dielectric constant and dielectric loss. This work therefore provides a possible strategy for the fabrication of thermal management polymers using 3D-printing methods.