Hierarchical lamellar single-walled carbon nanotube aerogel interlayers for stable lithium-sulfur batteries with high-sulfur-loading.

[Display omitted] • Single-walled carbon nanotube aerogels with hierarchical lamellar structures and a super-wettability are prepared by freeze casting for suppressing the shuttling of polysulfides in lithium-sulfur batteries. • The lithium-sulfur batteries with aerogel interlayers show a high initial area capacity of 7.1 mAh cm−2 at a sulfur loading of 8.02 mg cm−2. • The lean-electrolyte lithium-sulfur batteries with aerogel interlayers can maintain a specific capacity of 559 mAh g−1 at a sulfur loading of 10.35 mg cm−2. Lithium-sulfur (Li-S) battery has been recognized as a new energy storage device with broad prospects because of its satisfactory specific capacity and theoretical energy density. Nevertheless, the shuttle effect of polysulfides seriously hinders the real applications of high-sulfur-loaded Li-S batteries. To remove the hurdle, hierarchical lamellar single-walled carbon nanotube aerogels (SWCNTAs) are herein fabricated and applied as multifunctional interlayers in Li-S batteries, which exhibit an initial area-specific capacity as high as 7.1 mAh cm−2 at a sulfur loading of 8.02 mg cm−2. The introduced SWCNTA interlayers can lower the internal resistance and suppress the shuttling of polysulfides by a layer-by-layer physical blocking mechanism. Moreover, owing to the super wettability of SWCNTAs, electrolytes with a dosage of 10 μL mg−1 could effectively wet and infiltrate the interlayers, rendering the lean-electrolyte Li-S batteries a high specific capacity of 559 mAh g−1 at a sulfur loading of 10.35 mg cm−2 after 60 cycles. This work presents an example for rationally designing the interlayers structures for high-sulfur loading batteries, which paves a stepping stone for the future commercialization of Li-S batteries. [ABSTRACT FROM AUTHOR]