Ever
increasing demand on high energy density batteries positions
sulfur as a very promising cathode material for next-generation energy
storage due to its high theoretical capacity of 1675 mAh/g. Electronically
sulfur is highly insulating, and therefore integration of a conducting
framework such as a carbon nanotube (CNT) scaffold with sulfur is
a key aspect of the cathode design. Despite numerous efforts dedicated
to S-CNT cathode development, increasing sulfur loading to above 1
mg/cm2 while maintaining the cycling stability of the Li–S
cell remains challenging. This could be partly due to the lack of
understanding of the spatial distribution of sulfur in the CNT matrix
and its location with respect to the morphology of the CNT scaffold.
We demonstrate herein that the sulfur has a hierarchical distribution
in the CNT cathode at high sulfur loading (>5 mg/cm2) spanning
multiple length scales (from nanometer to submillimeter). Sulfur infiltration
into the CNT rather than the sulfur loading plays a key role in determining
the redox reaction kinetics, Li+ ion diffusion, and the
galvanostatic cycling capacity and stability of Li–S cells.
This study provides new insights for the design and fabrication of
high loading, binder-free sulfur–carbon-based cathode architectures
for next-generation high energy Li–S batteries.