Abstract

The rapidly growing market of portable and wearable smart electronics has created strong interest in flexible electrode materials with high specific capacitance and fast charging/discharging properties. However, high mass-specific capacitance active materials are often limited by the low areal mass-loading required. High areal capacity electrodes can make more efficient use of the limited internal space of these miniature devices by minimizing the volume and weight taken by current collectors and separators. Herein, a method is proposed to prepare a nickel–cobalt layered double hydroxide binder-free cathode on flexible carbon cloth with a mass loading of 20 mg cm−2. This core–shell hybrid structure prepared using a MOF self-sacrificing template, achieves a high energy density using thick electrodes while improving their slow kinetics by enhancing both the ion diffusion process and charge transfer dynamics. The areal capacitance reaches a staggering 4.42 mAh cm−2 (31.79 F cm−2) at a current density of 8 mA cm−2. Furthermore, a one-step hydrothermal method to prepare the FeNi-S anode (1.67 mAh cm−2, 2 mA cm−2) is proposed. Upon assembling with the gel electrolyte, this flexible device possesses an impressive energy density of 3.29 mW h cm−2 (3 mW cm−2). It can readily supply energy to watches, wireless e-paper, LEDs, and can be anticipated to be widely used in next-generation high-performance portable and wearable devices.

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