Flexible CNT-Interpenetrating Hierarchically Porous Sulfurized Polyacrylonitrile (CIHP-SPAN) Electrodes for High-Rate Lithium-Sulfur (Li-S) Batteries.

Sulfurized polyacrylonitrile (SPAN) is a promising cathode material for lithium-sulfur batteries owing to its reversible solid-solid conversion for high-energy-density batteries. However, the sluggish reaction kinetics of SPAN cathodes significantly limit their output capacity, especially at high cycling rates. Herein, a CNT-interpenetrating hierarchically porous SPAN electrode is developed by a simple phase-separation method. Flexible self-supporting SPAN cathodes with fast electron/ion pathways are synthesized without additional binders, and exceptional high-rate cycling performances are obtained even with substantial sulfur loading. For batteries assembled with this special cathode, an impressive initial discharge capacity of 1090 mAh g and a retained capacity of 800 mAh g are obtained after 1000 cycles at 1 C with a sulfur loading of 1.5 mg cm. Furthermore, by incorporating VO anchored carbon fiber as an interlayer with adsorption and catalysis function, a high initial capacity of 614.8 mAh g and a notable sustained capacity of 500 mAh g after 500 cycles at 5 C are achieved, with an ultralow decay rate of 0.037% per cycle with a sulfur loading of 1.5 mg cm. The feasible construction of flexible SPAN electrodes with enhanced cycling performance enlists the current processing as a promising strategy for novel high-rate lithium-sulfur batteries and other emerging battery electrodes.