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 Ti3C2T
x
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
Ti3C2T
x
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-Ti3C2T
x
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.