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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]

CeCoS x -SA/GF porous aerogels are fabricated based on sodium alginate with "egg-box" model and exhibited superior electrochemical properties as well as high mechanical strength. [Display omitted] • CeCoS x -SA/GF aerogels with "egg-box" structure is synthesized. • The CeCoS x -SA/GF electrode exhibits great electrochemical properties. • A portable multifunctional instrument can be powered for 28 mins. • Flexible CeCoS x -SA/GF/KOH/PVA film can be bent and twisted. • The CeCoS x -SA/GF/KOH/PVA film can lift 1 kg plastic bottle. Practical applications of flexible electrochemical energy storage devices are still limited by the lack of robust mechanical structures and high capacitive storage capabilities. Herein, the 3D CeCoS x -SA/GF porous aerogels are designed and prepared based on sodium alginate, which possess a special structure that can be explained by the so-called "egg-box" model. Each metal ion can be paired with the carboxyl and hydroxyl groups of the G monomer on two adjacent sodium alginate molecular chains. Melamine foam is used as carrier for graphene/sodium alginate impregnation and plays an important role on significantly limiting the agglomeration of graphene nanosheets due to their strong π-π stacking. The fabricated electrode based on CeCoS x -SA/GF shows an excellent electrochemical capacitance of 873.3F/g at the current density of 1A/g. In addition, the capacitance retention rate can still remain 87.1 % after 5000 cycles at a high current density of 8 A/g. Moreover, the fabricated all-solid state asymmetric supercapacitor device assembled with CoCeS x -SA/GF and active carbon shows an energy density of 29.58 Wh kg−1 at a power density of 801 W kg−1. For practical applications, the fabricated supercapacitor device can power a multifunctional display for 28 mins and illuminate a small light bulb for 3 mins. Moreover, the KOH/polyvinyl alcohol gel-electrolyte was used to fabricate high-strength and flexible CeCoS x -SA/GF/PVA/KOH composite film electrode, which can be bent at various angles (0°-180°) and can be twisted into various shapes. Notably, the CeCoS x -SA/GF/PVA/KOH composite film can lift plastic bottles containing 500 mL (500 g) and 1000 mL (1 kg) water, respectively, indicating that it has great application potential for wearable and portable electronic devices. [ABSTRACT FROM AUTHOR]