Localized Electron Density Regulation Effect for Promoting Solid–Liquid Ion Adsorption to Enhance Areal Capacitance of Micro‐Supercapacitors

The development of flexible microelectronic systems requires the construction of high-energy-output planar micro-supercapacitors (MSCs). Herein, the localized electron density, by introducing graphene quantum dots (GQDs) on the surface of electrodes, is regulated. The enhanced local field intensity promotes ion electrostatic adsorption at the solid-liquid interface, which significantly improves the energy density of MSCs in the confined space. Local electronic structure has been investigated from the perspective of the topological analysis of the electron localization function (ELF) and the electron density. Impressively, the edges of the simulated structure exhibit a higher electron density distribution than the CC skeleton. This finding indicates that the introduced GQDs reinforce the intrinsic electrical double-layer capacitance (EDLC) and the oxygen-bearing functional groups at the edge, further increasing the pseudocapacitance performance. Moreover, the edge electron aggregation effect enables the all-carbon-based symmetric MSCs to exhibit ultra-high areal capacitance (21.78 mF cm-2 ) and excellent cycle stability (86.74% retention after 25 000 cycles). This novel surface local charge regulation strategy is also applied for intensifying ion electrostatic adsorption on Zn-ion hybrid MSCs (polyvalent metal ions) and ion-gel electrolyte MSCs (non-metallic ions). With excellent planar integration, this device demonstrates excellent flexibility and has potential applications in timing and environmental monitoring.