Hierarchical NiCo2O4@NiMoO4 core–shell nanowire/nanosheet arrays were successfully fabricated and assembled in an asymmetric supercapacitor device with outstanding electrochemical performance.

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Nickel-based layered hydroxides (LDHs) have aroused much interest as promising battery-type electrodes for hybrid supercapacitors (HSCs) because of their high theoretical capacity, good safety, and abundant natural resources; however, the electrochemical performances are still notoriously limited owing to their intrinsically poor electrical conductivity and severe agglomeration features. Herein, an elaborate hierarchical NiCo 2 S 4 @NiCu−LDH nanotube/nanosheet hybrid electrode is designed and fabricated directly on carbon cloth by a facile multistep solution-based strategy. Through the rational engineering of nanostructures and atomic substitution of nickel by copper, the optimized NiCo 2 S 4 @NiCu−LDH hybrid electrode can yield a high areal capacity of 632.0 μAh/cm 2 at a current density of 2 mA/cm 2 and a good rate capability. Furthermore, the assembled flexible solid-state HSC device employing the NiCo 2 S 4 @NiCu−LDH exhibits a maximum volumetric energy density of 2.7 mWh/cm 3 at a power density of 21.3 mW/cm 3 with a robust long-term cycling stability over 2000 cycles and outstanding flexibility under repeated bending tests. Our work demonstrates the possibility of designing and fabricating nickel-based LDHs as superior battery-type electrodes towards highly durable and efficient flexible energy storage devices.

In this work, we report the design and fabrication of hierarchical NiCo2S4@polypyrrole (PPy) core–shell hybrid nanosheet arrays as a novel battery-type electrode for high-performance hybrid supercapacitors.

One-step sulfuration synthesis of NiCo2S4@NiCo2S4 core–shell arrays on carbon cloth.

Hierarchical NiCo2S4@NiMoO4 nanotube/nanosheet arrays were successfully fabricated on Ni foam as battery-type electrodes for high-performance hybrid supercapacitors.

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