LAUSR

The high solubility of the small organic molecule materials in organic electrolytes hinders their development in rechargeable batteries. Hence, this work designs an ultrarobust hydrogen-bonded organic-inorganic hybrid material: the small organic unit of the 1,3,6,8-tetrakis (p-benzoic acid) pyrene (TBAP) molecule connected with the hydroxylated Ti3C2Tx MXene through hydrogen bonds between the terminal groups of -COOH and -OH. The robust and elastic hydrogen bonds can empower the TBAP, despite being a low-molecule organic chemical, with unusually low solubility in organic electrolytes and thermal stability. The alkali-treated Ti3C2Tx MXene provides a hydroxyl-rich conductive network, and the small organic molecule of TBAP reduces the restacking of MXene layers. Therefore, the combination of these two materials complements each other well, and this organic-inorganic TBAP@D-Ti3C2Tx electrode delivers large reversible capacities and long cyclic life. Notably, with the assistance of the in situ FT-IR characterization of the electrode within the fully lithiated (0.005 V) and the delithiated (3.0 V) states, it is revealed that a powerful π-Li cation effect mainly governs the lithium-storage mechanism with the highly activated benzene ring and each C6 aromatic ring, which can reversibly accept six Li-ions to form a 1:1 Li/C complex.