Aqueous aluminum‐ion batteries (AABs) are regarded as promising next‐generation energy storage devices, and the current reported cathodes for AABs mainly focused on inorganic materials which usually implement a typical Al3+ ions (de)insertion mechanism. However, the strong electrostatic forces between Al3+ and the host materials usually lead to sluggish kinetics, poor reversibility and inferior cycling stability. Herein, we employ an organic compound with redox‐active moieties, phenazine (PZ), as the cathode material in AABs. Different from conventional inorganic materials confined by limited lattice spacing and rigid structure, the flexible organic molecules allow a large‐size Al‐complex co‐intercalation through reversible redox active centers (‐C=N‐) of PZ. This co‐intercalation behavior can effectively reduce desolvation penalty, and substantially lower the Coulombic repulsion during the ion (de)insertion process. Consequently, this organic cathode exhibits a high capacity and excellent cyclability, which exceeds those of most reported electrode materials for AABs. This work highlights the anion co‐intercalation chemistry of redox‐active organic materials, which is expected to boost the development of high‐performance multivalent‐ion battery systems.
Aqueous zinc‐ion batteries (ZIBs) are a promising candidate for fast‐charging energy‐storage systems due to its attractive ionic conductivity of water‐based electrolyte, high theoretical energy density, and low cost. Current strategies toward high‐rate ZIBs mainly focus on the improvement of ionic or electron conductivity within cathodes. However, enhancing intrinsic electrochemical reaction kinetics of active materials to achieve fast Zn2+ storage has been greatly omitted. Herein, for the first time, stable radical intermediate generation is demonstrated in a typical organic electrode material (methylene blue [MB]), which effectively decreases the reaction energy barrier and enhances the intrinsic kinetics of MB cathode, enabling ultrafast Zn2+ storage. Meanwhile, anionic co‐intercalation essentially avoids MB molecules rearranging their configuration and sharing Zn2+ with adjacent functional groups, thus keeps the structure stable. As a result, Zn–MB batteries exhibit an excellent rate capability up to 500C and ultralong life of 20 000 cycles with a negligible 0.07% capacity decay per cycle at 100C, which is superior to that of most reported aqueous ZIBs batteries. This work provides a novel strategy of stable radical chemistry for ultrafast‐charging aqueous ZIBs, which can be introduced to other appropriate organic materials and multivalent ion battery systems.
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