Immobilizing Redox-Active Tricycloquinazoline into a 2D Conductive Metal-Organic Framework for Lithium Storage

Heteroaromatic-conjugated aromatic molecules have inspired numerous interests in rechargeable batteries like Li-ion batteries, but were limited by low conductivity and easy dissolution in electrolytes. Herein, we immobilize a nitrogen-rich aromatic molecule tricycloquinazoline (TQ) and CuO₄ unit into a two-dimensional (2D) conductive metal-organic framework (MOF) to unlock their potential for Li⁺ storage. TQ was identified redox activity with Li⁺ for the first time. With a synergistic effect of TQ and CuO₄ unit, the 2D conductive MOF, named Cu-HHTQ (HHTQ=2,3,7,8,12,13-hexahydroxytricycloquinazoline), can facilitate the Li⁺ /e^- transport and ensure a resilient electrode, resulting in a high capacity of 657.6 mAh g^-1 at 600 mA g^-1 with extraordinary high-rate capability and impressive cyclability. Our findings highlight an efficient strategy of constructing electrode materials for energy storage with combining multiple redox-active moieties into conductive MOFs.