3D Architecting triple gradient graphene-based fiber electrode for high-performance asymmetric supercapacitors

High-performance fibrous architectures and controllable fabrication methods for active nanomaterials are fundamental in the development of fiber-based supercapacitors (FSCs). Herein, we rationally designed a triple gradient structured fibrous electrode based on three-dimensional (3D) architectural approach with Ni3S2 nanoflakes (Ni3S2 NFs) in situ growth on Ni-coated graphene fiber (Ni3S2-NiGFs) for highly energy-dense asymmetric supercapacitors. Remarkably, the Ni-metal coating imparted the Ni3S2-NiGFs exceptional electrical conductivity (619.8 S cm-1), mechanical strength (335.0 MPa), and flexibility without significantly compromising its density. Moreover, the unique 3D interconnected ultrathin Ni3S2 NFs significantly increase the contact area between the electrode and the electrolyte solution, providing abundant redox activity to facilitate ion transport and accumulation. Therefore, the fibrous electrode showcased a remarkable areal specific capacitance of 1387.6 mF cm-2 at 3 mA cm-2 in 3 M KOHaq electrolyte, while its asymmetric FSCs delivered an impressive areal energy density of 15.6 mu W h cm-2 at power density of 1.0 mW cm-2 along with durable cycle life (86.7 % of the initial specific capacitance retention over 10,000 cycles). In summary, the featured work provides a facile but robust electrode design to realize highly energy-dense flexible energy storage devices for next-generation wearable industries.