Broader applications of carbon nanotubes to real-world problems have largely gone unfulfilled because of difficult material synthesis and laborious processing. We report high-performance multifunctional carbon nanotube (CNT) fibers that combine the specific strength, stiffness, and thermal conductivity of carbon fibers with the specific electrical conductivity of metals. These fibers consist of bulk-grown CNTs and are produced by high-throughput wet spinning, the same process used to produce high-performance industrial fibers. These scalable CNT fibers are positioned for high-value applications, such as aerospace electronics and field emission, and can evolve into engineered materials with broad long-term impact, from consumer electronics to long-range power transmission.O n the molecular level, carbon nanotubes (CNTs) have an outstanding combination of mechanical strength and stiffness, electrical and thermal conductivity, and low density, making them ideal multifunctional materials that combine the best properties of polymers, carbon fibers, and metals (1). However, such outstanding properties have remained elusive on a macroscopic scale. Handling CNTs with sufficient length, stiffness, and chemical inertness introduces major challenges in material processing. Here we report lightweight fibers that approach the high specific strength of polymeric and carbon fibers, while also achieving the high specific electrical conductivity of metals and the specific thermal conductivity of graphite fibers.Two distinct routes have been developed for manufacturing neat CNT fibers (2). One route employs a solid-state process wherein CNTs are either directly spun into a fiber from the synthesis reaction zone (3, 4) or from a CNT forest grown on a solid substrate (5). This approach does not lend itself to the typical easy scale-up of chemical processes, as it combines multiple steps into a single one, limiting the options for process and material optimization. Indeed, solidstate fibers have low packing and poor orientation, and include impurities within their structure (6). Despite these shortcomings, solid-state CNT fibers have delivered the best properties so far (3, 4, 7-9). The reason for this relative success is the length of the CNTs that constitute these fibers-1 mm or more (2). Longer CNTs reduce the number of CNT ends in a fiber, yielding greater strength (10) and reducing CNT junctions, which increases electrical and thermal conductivity (11). The alternate fiber production route-wet spinning-was the first method for producing CNT fibers (12). In this process, premade CNTs are dissolved or dispersed in a fluid, extruded out of a spinneret, and coagulated into a solid fiber by extracting the dispersant. Wet spinning is easily scaled to industrial levels and is indeed the route by which highperformance fibers are manufactured (including ballistic fibers such as Kevlar and Twaron and structural fibers such as Toho Tenax and Thornel carbon fibers) (13). Decoupling the synthesis of CNTs from the spinning of the fibers allo...
Transparent conductive carbon nanotube (CNT) films were fabricated by dip-coating solutions of pristine CNTs dissolved in chlorosulfonic acid (CSA) and then removing the CSA. The film performance and morphology (including alignment) were controlled by the CNT length, solution concentration, coating speed, and level of doping. Using long CNTs (∼10 μm), uniform films were produced with excellent optoelectrical performance (∼100 Ω/sq sheet resistance at ∼90% transmittance in the visible), in the range of applied interest for touch screens and flexible electronics. This technique has potential for commercialization because it preserves the length and quality of the CNTs (leading to enhanced film performance) and operates at high CNT concentration and coating speed without using surfactants (decreasing production costs).
We study how intrinsic parameters of carbon nanotube (CNT) samples affect the properties of macroscopic CNT fibers with optimized structure. We measure CNT diameter, number of walls, aspect ratio, graphitic character, and purity (residual catalyst and non-CNT carbon) in samples from 19 suppliers; we process the highest quality CNT samples into aligned, densely packed fibers, by using an established wet-spinning solution process. We find that fiber properties are mainly controlled by CNT aspect ratio and that sample purity is important for effective spinning. Properties appear largely unaffected by CNT diameter, number of walls, and graphitic character (determined by Raman G/D ratio) as long as the fibers comprise thin few-walled CNTs with high G/D ratio (above ∼20). We show that both strength and conductivity can be improved simultaneously by assembling high aspect ratio CNTs, producing continuous CNT fibers with an average tensile strength of 2.4 GPa and a room temperature electrical conductivity of 8.5 MS/m, ∼2 times higher than the highest reported literature value (∼15% of copper's value), obtained without postspinning doping. This understanding of the relationship of intrinsic CNT parameters to macroscopic fiber properties is key to guiding CNT synthesis and continued improvement of fiber properties, paving the way for CNT fiber introduction in large-scale aerospace, consumer electronics, and textile applications.
Two types of graphene oxide fibers are spun from high concentration aqueous dopes. Fibers extruded from large flake graphene oxide dope without drawing show unconventional 100% knot efficiency. Fibers spun from small sized graphene oxide dope with stable and continuous drawing yield in good intrinsic alignment with a record high tensile modulus of 47 GPa.
We report that chlorosulfonic acid is a true solvent for a wide range of carbon nanotubes (CNTs), including single-walled (SWNTs), double-walled (DWNTs), multiwalled carbon nanotubes (MWNTs), and CNTs hundreds of micrometers long. The CNTs dissolve as individuals at low concentrations, as determined by cryo-TEM (cryogenic transmission electron microscopy), and form liquid-crystalline phases at high concentrations. The mechanism of dissolution is electrostatic stabilization through reversible protonation of the CNT side walls, as previously established for SWNTs. CNTs with highly defective side walls do not protonate sufficiently and, hence, do not dissolve. The dissolution and liquid-crystallinity of ultralong CNTs are critical advances in the liquid-phase processing of macroscopic CNT-based materials, such as fibers and films.
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