Vanadium oxyhydroxide has been recently
investigated as a starting
material to synthesize different phases of vanadium oxides by electrochemical
or thermal conversion and has been used as an aqueous zinc-ion battery
(AZIB) cathode. However, the low-valent vanadium oxides have poor
phase stability under ambient conditions. So far, there is no study
on understanding the phase evolution of such low-valent vanadium oxides
and their effect on the electrochemical performance toward hosting
the Zn2+ ions. The primary goal of the work is to develop
a high-performance AZIB cathode, and the highlight of the current
work is the insight into the auto-oxidation-induced phase transition
of VOOH to V10O24·nH2O under ambient conditions and Zn2+ intercalation
behavior thereon as an aqueous zinc-ion battery cathode. Herein, we
demonstrate that hydrothermally synthesized VOOH undergoes a phase
transition to V10O24·nH2O during both the electrochemical cycling and aerial
aging over 38–45 days. However, continued aging till 150 days
at room temperature in an open atmosphere exhibited an increased interlayer
water content in the V10O24·nH2O, which was associated with a morphological change
with different surface area/porosity characteristics and notably reduced
charge transfer/diffusion resistance as an aqueous zinc-ion battery
cathode. Although the fresh VOOH cathode had impressive specific capacity
at rate performance, (326 mAh/g capacity at 0.1 A/g current and 104
mAh/g capacity at 4 A/g current) the cathode suffered from a continuous
capacity decay. Interestingly, the aged VOOH electrodes showed gradually
decreasing specific capacity with aging at low current and however
followed the reverse order at high current. At a comparable specific
power of ∼64–66 W/kg, the fresh VOOH and aged VOOH after
60, 120, and 150 days of aging showed the respective energy densities
of 208.3, 281.2, 269.2, and 240.6 Wh/kg. Among all the VOOH materials,
the 150 day-aged VOOH cathode exhibited the highest energy density
at a power density beyond 1000 W/kg. Thanks to the improved kinetics,
the 150 day-aged VOOH cathode delivered a considerable energy density
of 39.7 Wh/kg with a high specific power of 4466 W/kg. Also, it showed
excellent cycling performance with only 0.002% capacity loss per cycle
over 20 300 cycles at 10 A/g.