Lithium–sulfur (Li–S)
batteries with their low cost,
high energy density, and theoretical specific capacity have been deemed
as one of the most promising candidates for the future energy storage
market. However, the insulating sulfur and the shuttling effect concerning
lithium polysulfides always persecute the sulfur cathode of Li–S
batteries. Consequently, a globular polypyrrole (PPy) interlayer (GPIL)
with multifunctional polysulfide-blocking ability wraps the carbon
aerogel/sulfur cathode to restrain this shuttling effect. Ultimately,
a high-performance Li–S battery is obtained through a polypyrrole
coating design. The maximum discharge specific capacity of the sulfur
cathode with a GPIL is 882 mAh g–1 at 1.4 mA cm–2 with the reversible specific capacity and an average
Coulombic efficiency of ∼652.7 mAh g–1 and
98.1%, respectively, after 100 cycles, indicating an effective impediment
of the shuttling effect. Moreover, the Li–S battery with a
GPIL can still deliver 520 mAh g–1 with a capacity
retention rate of >96% after 100 cycles at a high current density
of 2.8 mA cm–2, significantly outstripping most
of the interlayers recently reported. This work highlights the meaning
of this multifunctional interlayer and also promotes the great application
potential of carbon aerogel as the host of the sulfur cathode for
Li–S batteries.