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. The 2D conductive metal–organic framework Cu‐HHTQ with multiple redox‐active sites originating from a nitrogen‐rich aromatic molecule tricycloquinazoline (TQ) and a CuO4 unit was designed for Li‐ion batteries with high capacity, extraordinary high‐rate capability and impressive cyclability. TQ was identified as redox‐active with Li+ for the first time.