Lightweight thermal interface materials based on hierarchically structured graphene paper with superior through-plane thermal conductivity

Graphene-based papers have recently triggered considerable interests in developing the application as thermal interface materials (TIMs) for addressing the interfacial heat transfer issue, but their low through-plane thermal conductivity (κ⊥), resulting from the layer-by-layer stacked architecture, limits the direct use as TIMs. Although various hybrid graphene papers prepared by combining the graphene sheets and the thermally conductive in­ sertions have been proposed to solve this problem, achieving a satisfactory κ⊥ higher than that of commercial TIMs (>5 W m−1 K−1) remains challenging. Here, a strategy aimed at the construction of heat pathways along the through-plane direction inside the graphene paper for achieving a high κ⊥ was demonstrated through the simultaneous filtration of graphene sheets with two different lateral sizes. The as-prepared graphene paper presented a hierarchical structure composed of loosely stacked horizontal layers formed by large graphene sheets, intercalated by a random arrangement of small graphene sheets. Due to the heat pathways formed by small graphene sheets along the through-plane direction, the hierarchically structured graphene paper exhibited an improved κ⊥ as high as 12.6 W m−1 K−1 after a common graphitization post-treatment. In the practical test, our proposed paper as an all-graphene TIM achieved an enhancement in cooling efficiency of ≈ 2.2 times compared to that of the state-of-the-art TIM, demonstrating its superior performance to meet the ever-increasing heat dissipation requirement.