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.
Organic
electrodes have been identified as promising energy-storage
materials for aqueous zinc-ion batteries (AZIBs). Small molecular
materials have ideal redox properties, high specific capacity, and
structural diversity, making them a category of cathode candidates
for AZIBs. However, the instability and dissolution during the extraction
and insertion of H+/Zn2+ limit their application
of the long-cycle stability for AZIBs. Herein, a small-molecule nanosheet
(NI-DAQ, ∼14 nm in thickness) with imide linkage is designed
and synthesized by the condensation of anthraquinones and anhydrides.
It not only inhibits the dissolution of monomer electrodes but also
boosts the reactivity and conductivity of the whole molecule by the
introduction of π-conjugated imide groups and extended aromatic
planes. Therefore, the NI-DAQ electrode obtains a large initial capacity
of 191.9 mA h g–1 at 50 mA g–1 and superior cyclability after 3000 cycles at 500 mA g–1 with a minor average capacity fading rate of 0.01% per cycle. Moreover,
in situ Fourier transform infrared (FT-IR) and ex situ X-ray photoelectron
spectroscopy (XPS) characterization techniques have been implemented
to investigate the redox mechanism of CO units in AZIBs for
the NI-DAQ electrode. Thus, a promising conductive molecule is developed
and explored in this paper, which can provide insights into the application
of organic materials in AZIBs.
Molybdenum disulfide (MoS2), with its unique two-dimensional nanostructure and high theoretical capacity, is considered a promising electrode for lithium-ion batteries (LIBs). However, the disadvantages of MoS2 electrodes include low electronic...
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