▎ 摘　　要

Vacuum filtration is a highly effective and easy scale-up approach and has been widely used to fabricate graphene monoliths, such as graphene paper and graphene frameworks for various applications. In general, the microstructure of filtrated monoliths exhibits layer-by-layer stacking of graphene sheets due to the directional flow-induced assembly process. In this work, we found that the horizontally oriented structure of filtrated graphene frameworks can be modulated to an approximately isotropic arrangement by lowering the lateral size of graphene sheets. This size-dependent microstructure transition from anisotropic to isotropic was further confirmed by measuring the in- and through-plane thermal conductivity of the graphene/epoxy composites with different arrangements of graphene frameworks as a filler. Optimally, we obtained an epoxy composite embedded with a quasi-isotropic graphene framework (QIGF) by a simple two-step process: vacuum filtration of small graphene sheets to obtain the framework followed by the infiltration of epoxy resin. Based on the interconnected graphene sheets with an approximately isotropic arrangement, QIGF provides heat channels of graphene-graphene along both the in- and through-plane directions within epoxy. With a low graphene loading of 5.5 wt%, QIGF/epoxy (QIGF/EP) presents in- and through-plane thermal conductivities of 10.0 and 5.4 W mK(-1), respectively, which are equivalent to approximate to 55 and 29 times higher than those of neat epoxy. As compared to the current graphene/epoxy composites prepared by various methods, our QIGF/EP has the highest thermal conductivity value with this level of filler loading. Our findings provide an insight for the development of polymer composites for thermal management applications in industry.