Sufficiently Enriched Dual‐Ion Batteries with Ferrocenyl Substituted Nickel(II) Norcorrole Organic Electrodes

Abstract Ferrocenyl‐substituted nickel(II) norcorrole and nickel(II) porphyrin (Fc 2 NiNc and Fc 2 NiPor, respectively) are prepared as active electrode materials for dual‐ion batteries, which enables the systematically study of aromaticity and antiaromaticity for organic electrode materials. Intrinsically, Fc 2 NiNc and Fc 2 NiPor electrodes have excellent electrochemical behaviors with dual ion interaction with Li cations and bis(fluorosulfonyl)amide [FSA] – inorganic anions from the ionic liquid electrolyte, inducing high capacities (259 mAh g −1 for Fc 2 NiNc and 200 mAh g −1 for Fc 2 NiPor). The dominance of pseudocapacitive charge storage is exhibited by the Fc 2 NiNc and Fc 2 NiPor electrodes giving rise to rapid charge‐discharge processes. Computational calculation conclusively demonstrates the mechanism of multi‐electron redox reaction resulting in high discharge capacities and aromatic stabilization energy toward achieving a stable long‐term cyclability over 1000 cycles at high current density. Furthermore, Li 4 Ti 5 O 12 /IL/Fc 2 NiNc cells exhibit high power and energy densities (234 Wh kg −1 at 118 W kg −1 ) and accomplish outstanding cyclability over 10 000 cycles. This work provides a strategy for designing robust organic electrode materials for dual‐ion batteries.