Manganese
oxides composed of various valence states Mn
x+ (x = 2, 3, and 4) have attracted
wide attention as promising electrode materials for asymmetric supercapacitor.
However, the poor electrical conductivity limited their performance
and application. Appropriate regulation content of Mn
x+ in mixed-valent manganese oxide can tune the electronic
structure and further improve their conductivity and performance.
Herein, we prepared manganese oxides with different Mn2+/Mn3+ ratios through an over-reduction (OR) strategy for
tuning the internal electron structure of mixed-valent manganese,
which could make these material oxides a good platform for researching
the structure–property relationships. The Mn2+/Mn3+ ratio of manganese oxide could be precisely tuned from 0.6
to 1.7 by controlling the amount of reducing agent for manipulating
the redox processes, where the manganese oxide electrode with the
most appropriate Mn2+/Mn3+ ratio, as 1.65 (OR4)
exhibits large capacitance (274 F g–1) and the assembling
asymmetric supercapacitors by combining OR4 (positive) and the commercial
activated carbon (as negative) achieved large 2.0 V voltage window
and high energy density of 27.7 Wh kg–1 (power density
of 500 W kg–1). The cycle lifespan of the OR4//AC
could keep about 92.9% after 10 000-cycle tests owing to the
Jahn–Teller distortion of the Mn(III)O6 octahedron,
which is more competitive compared to other work. Moreover, a red-light-emitting
diode (LED) can easily be lit for 15 min by two all-solid supercapacitor
devices in a series.