ABSTRACT
Stretchable energy storage systems are essential for the realization of implantable and epidermal electronics. However, high-performance stretchable supercapacitors have received less attention because currently available processing techniques and material structures are too limited to overcome the trade-off relationship among electrical conductivity, ion-accessible surface area, and stretchability of electrodes. Herein, we introduce novel 2D reentrant cellular structures of porous graphene/CNT networks for omnidirectionally stretchable supercapacitor electrodes. Reentrant structures, with inwardly protruded frameworks in porous networks, were fabricated by the radial compression of vertically aligned honeycomb-like rGO/CNT networks, which were prepared by a directional crystallization method. Unlike typical porous graphene structures, the reentrant structure provided structure-assisted stretchability, such as accordion and origami structures, to otherwise unstretchable materials. The 2D reentrant structures of graphene/CNT networks maintained excellent electrical conductivities under biaxial stretching conditions and showed a slightly negative or near-zero Poisson's ratio over a wide strain range because of their structural uniqueness. For practical applications, we fabricated all-solid-state supercapacitors based on 2D auxetic structures. A radial compression process up to 1/10th densified the electrode, significantly increasing the areal and volumetric capacitances of the electrodes. Additionally, vertically aligned graphene/CNT networks provided a plentiful surface area and induced sufficient ion transport pathways for the electrodes. Therefore, they exhibited high gravimetric and areal capacitance values of 152.4 F g-1 and 2.9 F cm-2, respectively, and had an excellent retention ratio of 88% under a biaxial strain of 100%. Auxetic cellular and vertically aligned structures provide a new strategy for the preparation of robust platforms for stretchable energy storage electrodes.
ABSTRACT
Electrochemical energy storage devices based on electric double layer capacitors (EDLCs) have received considerable attention due to their high power density and potential for obtaining improved energy density in comparison to the lithium ion battery. Ordered mesoporous carbon (OMC) is a promising candidate for use as an EDLC electrode because it has a high specific surface area (SSA), providing a wider charge storage space and size-controllable mesopore structure with a long-range order, suppling high accessibility to the electrolyte ions. However, OMCs fabricated using conventional methods have several drawbacks including low electronic conductivity and long ionic diffusion paths in mesopores. We used nickel nanofoam, which has a relatively small pore (sub-100 nm to subµm) network structure, as a current collector. This provides a significantly shortened electronic/ionic current paths and plentiful surface area, enabling stable and close attachment of OMCs without the use of binders. Thus, we present hierarchical binder-free electrode structures based on OMC/Ni nanofoams. These structures give rise to enhanced specific capacitance and a superior rate capability. We also investigated the mesopore structural effect of OMCs on electrolyte transport by comparing the capacitive performances of collapsed lamellar, cylindrical, and spherical mesopore electrodes. The highly ordered and straightly aligned cylindrical OMCs exhibited the highest specific capacitance and the best rate capability.
