Graphene fiber-based supercapacitors (GFSCs) hold high power density, fast charge-discharge rate, ultralong cycling life, exceptional mechanical/electrical properties, and safe operation conditions, making them very promising to power small wearable electronics. However, the electrochemical performance is still limited by the severe stacking of graphene sheets, hydrophobicity of graphene fibers, and complex preparation process. In this work, we develop a facile but robust strategy to easily enhance electrochemical properties of all-solid-state GFSCs by simple plasma treatment. We find that 1 min plasma treatment under an ambient condition results in 33.1% enhancement of areal specific capacitance (36.25 mF/cm) in comparison to the as-prepared GFSC. The energy density reaches 0.80 μW h/cm in polyvinyl alcohol/HSO gel electrolyte and 18.12 μW h/cm in poly(vinylidene difluoride)/ethyl-3-methylimidazolium tetrafluoroborate electrolyte, which are 22 times of that of as-prepared ones. The plasma-treated GFSCs also exhibit ultrahigh rate capability (69.13% for 40 s plasma-treated ones) and superior cycle stability (96.14% capacitance retention after 20 000 cycles for 1 min plasma-treated ones). This plasma strategy can be extended to mass-manufacture high-performance carbonaceous fiber-based supercapacitors, such as graphene and carbon nanotube-based ones.

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Carbon nanomaterials are desirable candidates for lightweight, highly conductive, and corrosion-resistant current collectors. However, a key obstacle is their weak interconnection between adjacent nanostructures, which renders orders of magnitude lower electrical conductivity and mechanical strength in the bulk assemblies. Here we report an "epitaxial welding" strategy to engineer carbon nanotubes (CNTs) into highly crystalline and interconnected structures. Solution-based polyacrylonitrile was conformally coated on CNTs as "nanoglue" to physically join CNTs into a network, followed by a rapid high-temperature annealing (>2800 K, overall ∼30 min) to graphitize the polymer coating into crystalline layers that also bridge the adjacent CNTs to form an interconnected structure. The contact-welded CNTs (W-CNTs) exhibit both a high conductivity (∼1500 S/cm) and a high tensile strength (∼120 MPa), which are 5 and 20 times higher than the unwelded CNTs, respectively. In addition, the W-CNTs display chemical and electrochemical stabilities in strong acidic/alkaline electrolytes (>6 mol/L) when potentiostatically stressing at both cathodic and anodic potentials. With these exceptional properties, the W-CNT films are optimal as high-performance current collectors and were demonstrated in the state-of-the-art aqueous battery using a "water-in-salt" electrolyte.

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