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A honeycomb-like structure nanocomposite composed of Ag nanoparticles doped NiMn-LDHs nanosheets shell and uniformly arranged Co 2 (OH) 2 CO 3 nanoneedles core shows promising electrochemical storage properties. [Display omitted] • Honeycomb-like CC@Co 2 CH/NM-LDH-Ag nanosheet arrays are synthesized on carbon cloth. • The hybrid of various active components provides abundant active sites and fast ion diffusion. • CC@Co 2 CH/NM-LDH-Ag is used to prepare binder-free electrodes and exhibits excellent electrochemical properties. • The assembled all-solid-state asymmetric supercapacitor shows high energy density and power density. Layered double hydroxides are considered promising electrode materials for the preparation of high-energy–density supercapacitors owing to their suitable microstructure and significant electrochemical properties. In this study, honeycomb-like NiMn-layered double-hydroxide (NiMn-LDH) nanosheet arrays with numerous electron/ion channels, a large number of active sites, considerable redox reversibility, and significant electrical conductivity were synthesized by combining Co 2 (OH) 2 CO 3 nanoneedle arrays with NiMn-LDH nanosheet arrays and Ag nanoparticles on a carbon cloth (CC) substrate through a hydrothermal strategy (CC@Co 2 CH/NM-LDH-Ag). The fabricated CC@Co 2 CH/NM-LDH-Ag binder-free electrode exhibited a high specific capacitance of 10,976 mF cm−2 (3092F/g, 1391.4C g−1) at 2 mA cm−2 (1 A/g), and a high capacitance retention of 93.2 % after 10,000 cycles at a current density of 20 mA cm−2. In addition, a solid-state asymmetric supercapacitor (ASC) device assembled using CC@Co 2 CH/NM-LDH-Ag as the cathode possessed an ultrahigh energy density of 68.85 Wh kg−1 at a power density of 722.6 W kg−1, and two fabricated ASC units in series were able to power a multifunctional display for more than 30 min. Therefore, this study provides a new approach for the design and synthesis of high-performance flexible electrodes. [ABSTRACT FROM AUTHOR]

The excellent electrical conductivity of graphene is due to its highly‐conjugated structures. Manipulation of the electronic and mechanical properties of graphene can be achieved by controlling the destruction of its in‐sheet conjugation system. Herein, we report the preparation of CoCeSx−SA@BPMW@RGO through π‐π stacking interactions at the molecular level. In this study, sodium alginate was reacted with Co2+ and Ce3+, and the composite was loaded onto a graphene surface. The graphene sheets were prepared using a bi‐pyrene terminated molecular wire (BPMW) to avoid re‐stacking of the grapheme sheets, thereby forming nanoscale spaces between sheets. The angle between the BPMW coplanar pyrene group and the phenyl group was 33.2°, and the graphene layer is supported in an oblique direction. Finally, a three‐dimensional porous composite was obtained after annealing and vulcanization. The obtained CoCeSx−SA@BPMW@RGO exhibited excellent electrical conductivity and remarkable cycle stability. When the current density was 1 A g−1, its specific capacitance was as high as 1004 F g−1. BPMW modifies graphene through the synergistic effect of π‐π stacking interaction and special structure to obtain excellent electrochemical performance. Moreover, a solid‐state asymmetric supercapacitor device was fabricated based on the synthesized CoCeSx−SA@BPMW@RGO hybrid, which exhibited a power density of 979 W kg−1 at an energy density of 23.96 Wh kg−1. [ABSTRACT FROM AUTHOR]