Prussian blue analogues (PBAs) are promising electrode candidates for aqueous batteries because the inevitable interstitial water is generally thought to have little impact on battery performance. Currently, mounting researches have focused on optimizing PBA properties by varying transition metal composition, but less attention has been paid to interstitial water, especially in alkali metal-ion deficient PBAs with large cavities. Here, we employ the water-rich K 0.01 Mn[Cr(CN) 6 ] 0.74 ·4.75H 2 O as the negative electrode to study the effect of interstitial water. It is found that during de-potassiation, the electrode undergoes dehydration, which negatively impacts kinetics, distorts structure, and raises charging potential. A cation-self-shielding strategy involving Dihydroxyacetone (DHA) in the electrolyte to secure the water-rich state is then proposed. The built 1.82 V all-Prussian blue aqueous K-ion battery delivers a high practical specific energy of ~76 Wh kg −1 over 1.5 V (based on the total mass of active materials in both electrodes). This study reveals the significance of interstitial water on the kinetics of PBA negative electrodes and promotes the exploration of water-containing electrodes to develop high-voltage aqueous rechargeable batteries for energy storage applications.
Reduced Graphene oxide coating is applied to CuCoHCF material to remove interstitial water at mild reaction environment, and the conductivity is increased without damage of crystal structure. Superior electrochemical performance is observed from the capacitor devices with electrodes made from this material, which is attributed to the decrease in space resistance resulting from intact crystal structure. The specific capacity of 120.2 F g −1 , energy density of 86.5 Wh kg −1 and power density of 4.3 kW kg −1 is achieved on Cu 0.66 Co 0.33 HCF@rGO//AC device. The specific capacity is 98% of starting value after 2000 cycles.