The
energy density of supercapacitors with carbon-based electrode
materials is generally restricted by their limited electric double-layer
capacitance (EDLC). The introduction of electroactive molecules to
acquire abundant pseudocapacitance represents an efficient way to
achieve a high-performance capacitor system. Herein, this work anchors
redox-active tetramino-benzoquinone (TABQ) with multiwalled carbon
nanotubes (MWCNTs) to form a composite (denoted as TABQ-MWCNTs). Due
to the strong π–π stacking and H-bonding interaction
between TABQ molecules and the MWCNT host, the TABQ-MWCNTs acquire
enhanced structural stability and shortened pathway for electrons/charges,
which facilitate their energy storage capability. Specifically, by
adjusting the mass ratio of TABQ to MWCNTs, the composite can attain
a high specific capacitance of 463 F g–1 at 1 A
g–1 compared to that of bare MWCNTs (17 F g–1). Theoretical calculations show that TABQ-MWCNTs
own a lower adsorption energy toward H+, suggesting its
better EDLC capability through charge accumulation. Moreover, in situ Fourier transform infrared spectroscopy (FTIR) and
Raman tests reveal that the TABQ molecules hosted on MWCNTs undergo
a reversible evolution of the quinone-to-phenol structure during the
discharging/charging process, further verifying its promising pseudocapacitance
through faradic reactions. In addition to the high capacitance, the
TABQ-MWCNT composite also exhibits good cyclability in a three-electrode
system, i.e., 76.8% of the initial capacitance is obtained after cycling
for 6000 times at 10 A g–1. An asymmetric supercapacitor
(ASC) of TABQ-MWCNTs//activated carbon achieves a high energy density
of 15.6 Wh kg–1 at a power density of 700 W kg–1. Moreover, it also shows a long-term cyclability
of 91.5% after 10,000 cycles at 5 A g–1.