Lithium sulfur batteries with a high energy density of
2600 Wh
kg–1 and theoretical specific capacity of 1675 mAh
g–1 have been regarded as the most promising candidate
for the next generation of high-energy storage devices. However, their
commercial application is hindered by the undesirable troubles of
rapid capacity fading, insulation of the products (Li2S/Li2S2), volume expansion, and low mass loading. Herein,
a three-dimensional holey CNT/sulfurized polyacrylonitrile (CNT@SPAN)
freestanding cathode has been fabricated by a one-step phase inversion
method, followed by sulfurization without any binders and current
collectors. The unique porous framework design with SPAN in situ encapsulating
CNT can effectively facilitate the transportation of ions and electrons,
and endure the volume expansion of sulfur during the reaction process.
Simultaneously, by combining electrochemical impedance analysis and
frontier molecular orbit theory, the initial activation mechanism
of the Li-SPAN battery was explored. In the initial state of cell
activation, Li+ occupies the carbon skeleton continuously
and irreversibly, which enhances the conductivity of the composites.
This work refreshes the current performance of Li-SPAN batteries with
a maximum areal capacity of 10.21 mAh cm–2 at an
ultrahigh mass loading of 7.5 mg cm–2, and an excellent
rate capacity of 761.7 mAh g–1 at 4 C, which provides
a promising method to make Li–S batteries to meet the requirements
of commercial application.