Transition-metal oxides show great promise as electrode
materials
for supercapacitors due to their ease of synthesis, affordability,
adequate redox stability, and high theoretical capacity. However,
their inherent poor electrical conductivity and sluggish reaction
kinetics typically lead to low specific capacity, reduced energy and
power density, and sluggish rate capability in energy storage devices.
In this study, we have re-engineered common Co3O4 using a controlled solution combustion method to enhance oxygen
vacancy within the oxide materials. We compared this approach with
other calcination-based preparation techniques. Notably, the solution
combustion-derived Co3O4 (SCS) exhibited the
most significant oxygen vacancy along with higher surface area and
smaller crystallite size compared to calcination-derived Co3O4 (CLS) and Co3O4 (ZIF). The Co3O4 (SCS)-modified electrode demonstrated a remarkable
specific capacitance of 688.3 F/g at a current density of 1 A/g in
a three-electrode electrochemical systemnearly four times
of Co3O4 (ZIF) (173.3 F/g). Furthermore, the
solid-state asymmetric supercapacitor constructed with Co3O4 (SCS) [Co3O4 (SCS) @ITO//ITO]
exhibited a specific capacitance of 232 F/g at a 1 A/g current density,
along with high energy densities across a wide range of power densities
(e.g., 93.12 Wh/kg at 848.2 W/kg and 79.07 Wh/kg at 4248.55 W/kg),
surpassing the performance of most reported hybrid supercapacitors.
As a proof-of-concept, we further improved the oxygen vacancy in Co3O4 (SCS) through H2 treatment, resulting
in reduced Co3O4 (SCS-R) with an enhanced specific
capacitance of 278 F/g, an energy density of 111.58 Wh/kg, and a power
density of 869.45 W/kg at a 1 A/g current density. This modified material
also demonstrated exceptional capacitive efficiency (90%) and Coulombic
efficiency (90.2%) retention even after 6000 cycles. Ultimately, this
report introduces a straightforward solution combustion synthesis
strategy for generating oxygen vacancies in metal oxides, holding
significant promise for enhancing their energy storage properties.