Abstract

Hierarchical nanoarchitectures with large void space, unique porous networks, and numerous active sites for advanced supercapacitor (SC) electrodes has attracted great attention in modern electronics. Herein, a novel strategy is established to rational design of hierarchical iron cobalt selenide (FexCo3-xSe4) with tunable nanostructure and morphology by adjusting the stoichiometric ration of Fe: Co in order to enhance the energy density of SCs. The optimal FeCo2Se4 nanosheet arrays (NAs) enhances the electrical conductivity, electroactive sites, and intrinsic reactivity, achieving an ultra-high specific capacity of ~398.5 mA h g−1 at a current density of 1 mA cm−2 with an exceptional rate capability (~304.2 mA h g−1 at a current density of 50 mA cm−2), and ultra-long cycle life (~98.2% retention after 10,000 cycles). Taking advantage of FeCo2Se4 NAs positive electrode, we have successfully assembled solid-state asymmetric SC (ASC) with Fe2O3@NG hydrogel as the negative electrode. Impressively, the solid-state ASC achieves high operating voltage window upto 1.6 V, and thus delivers ultrahigh energy density of ~84.1 Wh kg−1 at a power density of 0.69 kW kg−1, and exceptional cycling stability (5.5% of capacity decay after 10,000 cycles), which outperform the recently reported metal selenide-based ASCs. These consequences clearly designate FeCo2Se4 NAs as an advanced electrode for next-generation energy storage technologies.

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