Advancing multifunctional thermal management with multistate graphene/CNTs conjugated hybrids

The formation of heat conduction pathway is the key to fulfill the demand for versatile thermal management. However, constructing a three-dimensional (3D) thermal bridge in a single step is challenging and entails the critical co-dispersion of multiple fillers. Here we propose a simple and controllable method to assemble conjugated hybrids of 1D carbon nanotubes (CNTs) with 2D graphene through hydrothermal centrifugation. In addition to armoring CNTs through the conjugation effect, ionic liquid crystals (ILC) assisted the CNTs to exfoliate graphite, facilitating the co-dispersion of the binary material. Remarkably, the resulting graphene/CNTs (GC) hybrids acquire hydrophilicity from the ILC and manifest diverse states depending on the water content, including octopus-like blocks, self-limiting gels, high-concentration slurries, and dilute dispersions. Hybrid nanocomposite papers containing ANF nanofibers with 3D thermally conductive bridges yield exceptional photothermal conversion performance and Joule heating performance, rendering them suitable for flexible wearable applications. The multistate GC hybrids presented here afford a novel reference for the one-step construction of 3D thermally conductive bridges.