Massive
efforts have been devoted to enhancing performances of
Li–S batteries to meet the requirements of practical applications.
However, problems remain in enhancing the energy density and improving
the cycle life. We present a free-standing structure of walnut-shaped
VS4 nanosites combine with carbon nanotubes (NTs) as cathodes.
In this framework, NT arrays provide high surface area and conductivity
for high sulfur loadings, and VS4 nanosites facilitate
trapping and catalytic conversions of lithium polysulfides. The synergistic
effects of free-standing NT arrays and VS4 nanosites have
enabled high rate capability up to 6 C and long-term cycling with
a low decay rate of 0.037% up to 1200 cycles at 2 C. Moreover, the
designed cathode can achieve high areal capacities up to ∼13
mAh·cm–2 and estimated gravimetric energy density
of 243.4 Wh·kg–1 at a system level, demonstrating
great potential in practical applications of Li–S batteries.