A carbon nanotube/molybdenum trioxide hybrid material
has been
developed in this contribution as a negative electrode for pseudocapacitors.
Molybdenum oxide was obtained by cathodic electrodeposition directly
on binder-free carbon nanotube mats, followed by annealing of the
electrode at 350 °C under air. The resulting pseudocapacitive
material has been characterized by scanning electron microscopy (SEM),
X-ray photoelectron spectroscopy (XPS), X-ray diffraction (XRD), Raman
spectroscopy, and electrochemistry. The effect of heat treatment on
the crystallinity and oxidation state of molybdenum oxide as well
as on electrochemical performances was investigated. By optimizing
the synthesis conditions, a maximum capacitance of up to 274 F/g has
been obtained at 2 mV/s in an organic electrolyte (LiTFSI/GBL 0.5
M) with high electroactive material loading and binder-free electrodes
(1 mg/cm2 with up to 75% of MoO3). A fully asymmetric
pseudocapacitor was then developed in association with a positive
pseudocapacitive hybrid electrode material based on MnO2 mixed with rGO/CNT mats. This MoO3–CNT||MnO2–rGO–CNT hybrid system, fabricated using industrially
suitable, nontoxic, and low-energy-consuming fabrication methods (dynamic
spray-gun deposition of an alcohol suspension followed by electrodeposition
in an aqueous electrolyte), showed a high energy density of 23 Wh/kg
with a power density of up to 100 W/kg. This system was able to maintain
energy densities higher than 10 Wh/kg for high power densities of
up to 4 kW/kg, proving that optimization of pseudocapacitive materials
through specific adaptations to organic electrolytes is viable. The
controlled nanostructuration and crystallization of the electrode
material and the complementary asymmetric configuration have important
beneficial effects on the performances of the global system.