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-1 and a retained capacity of 800 mAh g-1 are obtained after 1000 cycles at 1 C with a sulfur loading of 1.5 mg cm-2. Furthermore, by incorporating V2O5 anchored carbon fiber as an interlayer with adsorption and catalysis function, a high initial capacity of 614.8 mAh g-1 and a notable sustained capacity of 500 mAh g-1 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-2. 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.

Highly stable lithium sulfur batteries enhanced by flocculation and solidification of soluble polysulfides in routine ether electrolyte.

Lithium-sulfur batteries (LSBs) are among the most promising next-generation high energy density energy-storage systems. However, practical application has been hindered by fundamental problems, especially shuttling by the higher-order polysulfides (PSs) and slow redox kinetics. Herein, a novel electrolyte-based strategy is proposed by adding an ultrasmall amount of the low-cost and commercially available cationic antistatic agent octadecyl dimethyl hydroxyethyl quaternary ammonium nitrate (SN) into a routine ether electrolyte. Due to the strong cation-anion interaction and bridge-bonding with SN, rapid flocculation of the soluble polysulfide intermediates into solid-state polysulfide-SN sediments is found, which significantly inhibited the adverse shuttling effect. Moreover, a catalytic effect was also demonstrated for conversion of the polysulfide-SN intermediates, which enhanced the redox kinetics of Li-S batteries. Encouragingly, for cells with only 0.1 % added SN, an initial specific capacity of 783.6 mAh/g and a retained specific capacity of 565.7 mAh/g were found at 2C after 200 cycles, which corresponded to an ultralow capacity decay rate of only 0.014 % per cycle. This work may provide a simple and promising regulation strategy for preparing highly stable Li-S batteries.