Capacitive energy storage has advantages of high power density, long lifespan, and good safety, but is restricted by low energy density. Inspired by the charge storage mechanism of batteries, a spatial charge density (SCD) maximization strategy is developed to compensate this shortage by densely and neatly packing ionic charges in capacitive materials. A record high SCD (ca. 550 C cm-3 ) was achieved by balancing the valance and size of charge-carrier ions and matching the ion sizes with the pore structure of electrode materials, nearly five times higher than those of conventional ones (ca. 120 C cm-3 ). The maximization of SCD was confirmed by Monte Carlo calculations, molecular dynamics simulations, and in situ electrochemical Raman spectroscopy. A full-cell supercapacitor was further constructed; it delivers an ultrahigh energy density of 165 Wh L-1 at a power density of 150 WL-1 and retains 120 Wh L-1 even at 36 kW L-1 , opening a pathway towards high-energy-density capacitive energy storage.
Keywords: capacitive energy storage; in situ Raman spectroscopy; ion sieving effect; spatial charge density; zinc ion hybrid capacitor.
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