Ether-compatible sulfurized polyacrylonitrile cathode with excellent performance enabled by fast kinetics via selenium doping.

Chen, Xin; Peng, Linfeng; Wang, Lihui; Yang, Jiaqiang; Hao, Zhangxiang; Xiang, Jingwei; Yuan, Kai; Huang, Yunhui et al. · Nat Commun · 2019

basic_science · Level V

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Abstract

Sulfurized polyacrylonitrile is suggested to contain S<sub>n</sub> (n ≤ 4) and shows good electrochemical performance in carbonate electrolytes for lithium sulfur batteries. However inferior results in ether electrolytes suggest that high solubility of Li<sub>2</sub>S<sub>n</sub> (n ≤ 4) trumps the limited redox conversion, leading to dissolution and shuttling. Here, we introduce a small amount of selenium in sulfurized polyacrylonitrile to accelerate the redox conversion, delivering excellent performance in both carbonate and ether electrolytes, including high reversible capacity (1300 mA h g<sup>-1</sup> at 0.2 A g<sup>-1</sup>), 84% active material utilization and high rate (capacity up to 900 mA h g<sup>-1</sup> at 10 A g<sup>-1</sup>). These cathodes can undergo 800 cycles with nearly 100% Coulombic efficiency and ultralow 0.029% capacity decay per cycle. Polysulfide dissolution is successfully suppressed by enhanced reaction kinetics. This work demonstrates an ether compatible sulfur cathode involving intermediate Li<sub>2</sub>S<sub>n</sub> (n ≤ 4), attractive rate and cycling performance, and a promising solution towards applicable lithium-sulfur batteries.