Three-Dimensional SiC/Holey-Graphene/Holey-MnO₂Architectures for Flexible Energy Storage with Superior Power and Energy Densities

Although nanostructured materials have recently enabled a dramatic improvement of the current energy-storage units in portable electronics with enhanced functionality, it is still challenging to provide a cost-efficient solution to attain the ultrahigh energy and power densities of supercapacitors (SCs) since nearly arbitrary electrodes are limited to the thinner porous structure with de facto rather low mass loading (∼1 mg cm-2) because of the huge limitations of pronounced impaired ion transport in subnanometer pores in thicker compact electrodes. In this contribution, we report the fabrication of a macro/mesoporous hybrid hierarchical nanocomposite SiC/holey-graphene/holey-MnO2 (SiC/HG/h-MnO2) with tailored porosity by knitting together the quasi-aligned single-crystalline doped 3C-SiC nanowire array and in situ surface-reduced holey graphene framework into a three-dimensional quasi-ordered structure, which enables the mass growth of ultrathin h-MnO2 nanosheets at approximately practical levels of mass loading. The produced synergistically favorable interconnected porous architecture allows for the highly efficient electron transfer and rapid ion transport up to interior surfaces of the network. Remarkably, the all-solid-state flexible asymmetric supercapacitors (ASCs) made with SiC/HG/h-MnO2 and SiC/graphitic carbon (GC) nanoarrays are mechanically robust and show a high areal capacity (0.32 mWh cm-2) and a high rate capability (280 mW cm-2) at ultrahigh mass loading (6.5 mg cm-2), much higher than most of previous superior SCs in aqueous or gelled electrolytes and thus offer an entirely new prototype of textile-based ASCs, which represents a critical step toward practical applications for various portable electronics.