Self-Assembled Multifunctional Hybrids: Toward Developing High-Performance Graphene-Based Architectures for Energy Storage Devices

The prospect of developing multifunctional flexible three-dimensional (3D) architectures based on integrative chemistry for lightweight, foldable, yet robust, electronic components that can turn the many promises of graphene-based devices into reality is an exciting direction that has yet to be explored. Herein, inspired by nature, we demonstrate that through a simple, yet novel solvophobic self-assembly processing approach, nacre-mimicking, layer-by-layer grown, hybrid composite materials (consisting of graphene oxide, carbon nanotubes, and conducting polymers) can be made that can incorporate many of the exciting attributes of graphene into real world materials. The as-produced, self-assembled 3D multifunctional architectures were found to be flexible, yet mechanically robust and tough (Young’s modulus in excess of 26.1 GPa, tensile strength of around 252 MPa, and toughness of 7.3 MJ m^–3), and exhibited high native electrical conductivity (38700 S m^–1) and unrivalled volumetric capacitance values (761 F cm^–3) with excellent cyclability and rate performance

Organic Solvent-Based Graphene Oxide Liquid Crystals: A Facile Route toward the Next Generation of Self-Assembled Layer-by-Layer Multifunctional 3D Architectures

We introduce soft self-assembly of ultralarge liquid crystalline (LC) graphene oxide (GO) sheets in a wide range of organic solvents overcoming the practical limitations imposed on LC GO processing in water. This expands the number of known solvents which can support amphiphilic self-assembly to ethanol, acetone, tetrahydrofuran, <i>N</i>-dimethylformamide, <i>N</i>-cyclohexyl-2-pyrrolidone, and a number of other organic solvents, many of which were not known to afford solvophobic self-assembly prior to this report. The LC behavior of the as-prepared GO sheets in organic solvents has enabled us to disperse and organize substantial amounts of aggregate-free single-walled carbon nanotubes (SWNTs, up to 10 wt %) without compromise in LC properties. The as-prepared LC GO-SWNT dispersions were employed to achieve self-assembled layer-by-layer multifunctional 3D hybrid architectures comprising SWNTs and GO with unrivalled superior mechanical properties (Young’s modulus in excess of 50 GPa and tensile strength of more than 500 MPa)

High-Performance Multifunctional Graphene Yarns: Toward Wearable All-Carbon Energy Storage Textiles

The successful commercialization of smart wearable garments is hindered by the lack of fully integrated carbon-based energy storage devices into smart wearables. Since electrodes are the active components that determine the performance of energy storage systems, it is important to rationally design and engineer hierarchical architectures atboth the nano- and macroscale that can enjoy all of the necessary requirements for a perfect electrode. Here we demonstrate a large-scale flexible fabrication of highly porous high-performance multifunctional graphene oxide (GO) and rGO fibers and yarns by taking advantage of the intrinsic soft self-assembly behavior of ultralarge graphene oxide liquid crystalline dispersions. The produced yarns, which are the only practical form of these architectures for real-life device applications, were found to be mechanically robust (Young’s modulus in excess of 29 GPa) and exhibited high native electrical conductivity (2508 ± 632 S m^–1) and exceptionally high specific surface area (2605 m² g^–1 before reduction and 2210 m² g^–1 after reduction). Furthermore, the highly porous nature of these architectures enabled us to translate the superior electrochemical properties of individual graphene sheets into practical everyday use devices with complex geometrical architectures. The as-prepared final architectures exhibited an open network structure with a continuous ion transport network, resulting in unrivaled charge storage capacity (409 F g^–1 at 1 A g^–1) and rate capability (56 F g^–1 at 100 A g^–1) while maintaining their strong flexible nature