Ternary layered double-hydroxide-based active compounds are regarded as ideal electrode materials for supercapacitors because of their unique structural characteristics and excellent electrochemical properties. Herein, an NiCeCo-layered double hydroxide with a core−shell structure grown on copper bromide nanowire arrays (CuBr 2 @NCC-LDH/CF) has been synthesized through a hydrothermal strategy and calcination process and utilized to fabricate a binder-free electrode. Due to the unique top-tangled structure and the complex assembly of different active components, the prepared hierarchical CuBr 2 @NCC-LDH/CF binder-free electrode exhibits an outstanding electrochemical performance, including a remarkable areal capacitance of 5460 mF cm −2 at 2 mA cm −2 and a capacitance retention of 88% at 50 mA cm −2 as well as a low internal resistance of 0.163 Ω. Moreover, an all-solid-state asymmetric supercapacitor (ASC) installed with CuBr 2 @NCC-LDH/CF and activated carbon electrodes shows a high energy density of 118 Wh kg −1 at a power density of 1013 W kg −1 . Three assembled ASCs connected in series can operate a multifunctional display for over three and a half hours. Therefore, this innovative work provides new inspiration for the preparation of electrode materials for supercapacitors.

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Transition-metal selenides (TMSs) have great potential in the synthesis of supercapacitor electrode materials due to their rich content and high specific capacity. However, the aggregation phenomenon of TMS materials in the process of charging and discharging will cause capacity attenuation, which seriously affects the service life and practical applications. Therefore, it is of great practical significance to design simple and efficient synthesis strategies to overcome these shortcomings. Hence, P-doped Cu3Se2 nanosheets are loaded on vertically aligned Cu2S nanorod arrays to synthesize CF/Cu2S@Cu3Se2/P nanocomposites with a unique core–shell heterostructure. Notably, the Cu2S precursors can be rapidly converted into Cu3Se2 nanorod arrays in situ in just 30 min at room temperature. The unique core–shell heterostructure effectively avoids the aggregation phenomenon, and the doped P elements further enhance the electrochemical properties of the electrode materials. Therefore, the as-prepared CF/Cu2S@Cu3Se2/P electrode exhibits a high areal capacitance of 5054 mF cm–2 (1099 C g–1) at 3 mA cm–2 and still retains 90.2% capacitance after 10 000 galvanostatic charge–discharge (GCD) cycles. The asymmetric supercapacitor (ASC) device assembled from synthetic CF/Cu2S@Cu3Se2/P and activated carbon (AC) possesses an energy density of 41.1 Wh kg–1 at a power density of 480.4 W kg–1. This work shows that the designed CF/Cu2S@Cu3Se2/P electrode has broad application prospects in the field of electrochemical energy storage.

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With the urgent demand for the achievement of carbon neutrality, novel nanomaterials, and environmentally friendly nanotechnologies are constantly being explored and continue to drive the sustainable development of energy storage and conversion installations. Among various candidate materials, metal‐organic frameworks (MOFs) and their derivatives with unique nanostructures have attracted increasing attention and intensive investigation for the construction of next generation electrode materials, benefitting from their unique intrinsic characteristics such as large specific surface area, high porosity, and chemical tunability as well as the interconnected channels. Nevertheless, the poor electrochemical conductivity severely limits their application prospects, hence a variety of nanocomposites with multifarious structures have been designed and proposed from different dimensionalities. In this review, recent advances based on MOFs and their derivatives in different dimensionalities ranging from 1D nanopowders to 2D nanofilms and 3D aerogels, as well as 4D self‐supporting electrodes for supercapacitors are summarized and highlighted. Furthermore, the key challenges and perspectives of MOFs and their derivatives‐based materials for the practical and sustainable electrochemical energy conversion and storage applications are also briefly discussed, which may be served as a guideline for the design of next‐generation electrode materials from different dimensionalities.

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