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

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

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摘要

Organic redox-active materials are promising electrode candidates for lithiumion 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.

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