Rechargeable calcium-ion batteries are intriguing alternatives for use as post-lithium-ion batteries. However, the high charge density of divalent Ca2+ establishes a strong electrostatic interaction with the hosting lattice, which results in low-capacity Ca-ion storage. The ionic radius of Ca2+ further leads to sluggish ionic diffusion, hindering high-rate capability performances. Here, we report 5,7,12,14-pentacenetetrone (PT) as an organic crystal electrode active material for aqueous Ca-ion

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... torage. The weak π-π stacked layers of the PT molecules render a flexible and robust structure suitable for Ca-ion storage. In addition, the channels within the PT crystal provide efficient pathways for fast ionic diffusion. The PT anode exhibits large specific capacity (150.5 mAh g-1 at 5 A g-1), high-rate capability (86.1 mAh g-1 at 100 A g-1) and favorable low-temperature performances. A mechanistic study identifies proton-assisted uptake/removal of Ca2+ in PT during cycling. First principle calculations suggest that the Ca ions tend to stay in the interstitial space of the PT channels and are stabilized by carbonyls from adjacent PT molecules. Finally, pairing with a high-voltage positive electrode, a full aqueous Ca-ion cell is assembled and tested.