Three-Dimensional Hierarchically Porous Graphene Fiber-Shaped Supercapacitors with High Specific Capacitance and Rate Capability

Chemically converted graphene fiber-shaped supercapacitors (FSSCs) are highly promising flexible energy storage devices for wearable electronics. However, the ultralow specific capacitance and poor rate performance severely hamper their practical applications. They are caused by severe stacking of graphene nanosheets and tortuous ion diffusion path in graphene-based electrodes; thus, the ultralow utilization of graphene has been rarely carefully considered to date. Here, we address these issues by developing three-dimensional hierarchically porous graphene fiber with the incorporation of holey graphene for efficient utilization of graphene to achieve fast charge diffusion and good charge storage capability. Without deterioration in electrical but robust mechanical properties, the optimal graphene fiber shows ultrahigh specific capacitance of 220.1 F cm–3 at current density of 0.1 A cm–3 and boosted specific capacitance of 254.3 F cm–3 at 0.1 A cm–3 after nitrogen doping. Moreover, the nitrogen-doped 40% holey graphene hybrid fiber-assembled FSSC exhibits ultrahigh rate capability (96, 91, and 87% at current density of 0.5, 1.0, and 2.0 A cm–3, respectively, and 67% even at ultrahigh current density of 10.0 A cm–3) and excellent cycle stability (95.65% capacitance retention after 10 000 cycles). The contribution of three-dimensional interconnected hierarchically porous network to the enhanced electrochemical (EC) performance is semiquantitatively elucidated by Brunauer–Emmett–Teller and energy dispersive spectroscopy mapping. Our work gives insights into the importance of fully utilizing graphene and provides an efficient strategy for high EC performance in chemically converted graphene-based FSSCs.