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.