Editable asymmetric all-solid-state supercapacitors based on high-strength, flexible, and programmable 2D-metal–organic framework/reduced graphene oxide self-assembled papers

Abstract

Although some progress has been made in flexible supercapacitors (SCs), their high energy density, mechanical robustness, and device-level editability and programmability are still highly desirable for the development of advanced portable and miniaturized electronics, especially considering the fact that these flexible devices are likely to experience some mechanical impact and potential damage. Herein, we demonstrate the fabrication of hybrid electrodes containing self-assembled 2D metal–organic framework (MOF)/reduced graphene oxide (rGO) papers, which not only efficiently alleviate the self-restacking of rGO and the MOF but also maintain high electrical conductivity (0.32 Ω cm), excellent flexibility and mechanical properties with a Young's modulus of 34.4 GPa and a tensile strength of 89.9 MPa. In addition, a one-for-two strategy is introduced to construct two types of porous electrodes for flexible asymmetric SCs via a one MOF-derived synthesis route with simply changing metal ion precursors. As a consequence, the flexible asymmetric SCs possess a high volumetric energy density of 1.87 mW h cm⁻³ and an outstanding volumetric power density of 250 mW cm⁻³. More importantly, the all-solid-state asymmetric SCs exhibit high editability and bending-tolerance properties and perform very well under various severe service conditions, such as being seriously cut, bent, and heavily loaded. Particularly, the operations of micro-SCs with artistically designed patterns are demonstrated. Being high-strength, easily programmable and connectable in series and in parallel, the editable supercapacitor is promising for developing stylish energy storage devices to power various portable, miniaturized, and wearable devices.