Controllable assembly of continuous hollow graphene fibers with robust mechanical performance and multifunctionalities

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Macroscopic conformation of individual graphene sheets serves as the backbone of translating their intrinsic merits towards multifunctional practical applications. However, controllable and continuous assemblies of graphene-based nanomaterials to create stable macroscopic structural components are always in face of great challenge. We have developed a scalable converging-flow assisted wet-spinning methodology for continuously fabricating hollow graphene fibers (HGFs, the newest variation of solid graphene fibers) with high quality. The degradable silk thread is selectively utilized as the continuous hollow structure former that holds the coaxially stacked graphene sheets aligned through the converging-flow modulating process. For the first time, we have created the longest freestanding HGF in length of 2.1 m. The continuous HGFs are in an average diameter of 180 μm and with 4–8 μm adjustable wall thicknesses. The optimal HGF demonstrates an average tensile strength of 300 MPa and modulus of 2.49 GPa (comparable to typical solid graphene fibers, but the highest among the reported HGFs in literature) and an exceptional failure elongation of 10.8%. Additionally, our continuous HGFs exhibit spontaneous resistive response to thermal and strain stimuli (in form of large deformations and human motions), offering great potential for developing multifunctional sensors. We envision that this work demonstrates an effective and well-controlled macroscopic assembly methodology for the scaled-up mass production of HGFs.