In this study, we investigated the synergistic effects of thermally conductive hybrid carbonaceous fillers of mesophase pitch-based carbon fibers (MPCFs) and reduced graphene oxides (rGOs) on the thermal conductivity of polymer matrix composites. Micro-sized MPCFs with different lengths (50 μm, 200 μm, and 6 mm) and nano-sized rGOs were used as the thermally conductive fillers used for the preparation of the heat-dissipation polymer composites. For all MPCF fillers with a different length, the thermal conductivity values of the MPCF/epoxy composites were proportional to the MPCF length and loading amount (0-50 wt%) of MPCFs. For an MPCF:rGO weight ratio of 49:1 (total loading amount of 50 wt%), the thermal conductivity values of MPCF-rGO/epoxy composites loaded with MPCFs of 50 μm, 200 μm, and 6 mm increased from 5.56 to 7.98 W/mK (approximately 44% increase), from 7.36 to 9.80 W/mK (approximately 33% increase), and from 11.53 to 12.58 W/mK (approximately 9% increase) compared to the MPCF/epoxy composites, respectively, indicating the synergistic effect on the thermal conductivity enhancement. The rGOs in the MPCF-rGO/epoxy composites acted as thermal bridges between neighboring MPCFs, resulting in the formation of effective heat transfer pathways. In contrast, the MPCF-rGO/epoxy composites with MPCF:rGO weight ratios of 48:2 and 47:3 decreased the synergistic effect more significantly compared to rGO content of 1 wt%, which is associated with the agglomeration of rGO nanoparticles. The synergistic effect was inversely proportional to the MPCF length. A theoretical approach, the modified Mori-Tanaka model, was used to estimate the thermal conductivity values of the MPCF-rGO/epoxy composites, which were in agreement with the experimentally measured values for MPCF-rGO/epoxy composites loaded with short MPCF lengths of 50 and 200 μm.
Keywords: heat dissipation; hybrid carbonaceous filler; mesophase pitch-based carbon fiber; polymer composite; reduced graphene oxide; thermal conductivity.