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Aggregation of two-dimensional (2D) nanosheet fillers in a polymer matrix is a prevalent problem when the filler loading is high, leading to degradation of physical and mechanical properties of the composite. To avoid aggregation, a low-weight fraction of the 2D material (<5 wt %) is usually used to fabricate the composite, limiting performance improvement. Here, we develop a mechanical interlocking strategy where well-dispersed high filling content (up to 20 wt %) of boron nitride nanosheets (BNNSs) can be incorporated into a polytetrafluoroethylene (PTFE) matrix, resulting in a malleable, easy-to-process and reusable BNNS/PTFE composite dough. Importantly, the well-dispersed BNNS fillers can be rearranged into a highly oriented direction due to the malleable nature of the dough. The resultant composite film has a high thermal conductivity (4408% increase), low dielectric constant/loss, and excellent mechanical properties (334%, 69%, 266%, and 302% increases for tensile modulus, strength, toughness, and elongation, respectively), making it suitable for thermal management applications in the high-frequency areas. The technique is useful for the large-scale production of other 2D material/polymer composites with a high filler content for different applications.

The violent reaction processing and required high-temperature environment involved in growing carbon onions make it difficult to obtain an insight into their evolution mechanism. By using deionized water as the medium of arc discharge, we successfully froze the synthetic reaction at intermediary stages and observed detailed structures of the obtained intermediates of carbon onions. Here we present the atomic-scale scanning transmission electron microscopy investigation of carbon onions produced by arc discharge in water. We directly observed that carbon onions at intermediary growth stage are characterized by unclosed few-layer graphene shells. Meanwhile, a kind of graphene flakes composed of 3 layers or less were also observed in the sample. The kindred evolution linkage was induced to exist among these few-layer graphene flakes and carbon onions in the arc discharge synthetic process. On the basis of microscopy observations, we propose that carbon onions are constructed by curling few-layer graphene flakes, which is beneficial for structural designs and controls of related carbon materials used in different fields.