The lithium-sulfur battery (LSB)
is a promising candidate for high-performance
energy storage applications due to its high theoretical energy density
and low cost. However, developing a highly durable sulfur cathode
for LSBs has been challenging due to the known polysulfide shuttling
and volume variation of sulfur that leads to chemical and mechanical
degradation of the cathode during cycling. Sulfur confinement has
become a promising solution to both issues. However, confining sulfur
typically requires a complex and expensive process. Herein, we present
a simple electrode processing method for producing highly durable
sulfur cathodes with self-structured binder confinement for sulfur
particles using only commercially available sulfur, carbon black,
and binder, with no additional components. The dissolution of the
binder is controlled during the slurry preparation step to form a
porous binder/carbon shell structure around the sulfur particles that
can entrap the soluble polysulfides and slow down the shuttling mechanism.
The sulfur cathodes achieved through this method offer an outstanding
capacity retention of 74% over 1000 cycles, a considerable reduction
in the lithium-polysulfide shuttling and active material loss. Electrodes
with a high areal loading of 7.37 mAh/cm2 (4.4 mg/cm2) also showed excellent cyclability as well as a high capacity
of 800 mAh/g. The simplicity and cost-effectiveness of the presented
method make it promising for the large-scale manufacturing of low-cost
and durable sulfur cathodes, which pave the path to the commercialization
of LSBs.