Stabilizing Redox‐Active Hexaazatriphenylene in a 2D Conductive Metal–Organic Framework for Improved Lithium Storage Performance

Abstract

Abstract Organic redox‐active materials are promising electrode candidates for lithium‐ion batteries by virtue of their designable structure and cost‐effectiveness. However, their poor electrical conductivity and high solubility in organic electrolytes limit the device's performance and practical applications. Herein, the π‐conjugated nitrogen‐containing heteroaromatic molecule hexaazatriphenylene (HATN) is strategically embedded with redox‐active centers in the skeleton of a Cu‐based 2D conductive metal–organic framework (2D c ‐MOF) to optimize the lithium (Li) storage performance of organic electrodes, which delivers improved specific capacity (763 mAh g −1 at 300 mA g −1 ), long‐term cycling stability (≈90% capacity retention after 600 cycles at 300 mA g −1 ), and excellent rate performance. The correlation of experimental and computational results confirms that this high Li storage performance derives from the maximum number of active sites (CN sites in the HATN unit and CO sites in the CuO 4 unit), favorable electrical conductivity, and efficient mass transfer channels. This strategy of integrating multiple redox‐active moieties into the 2D c ‐MOF opens up a new avenue for the design of high‐performance electrode materials.