Switchable encapsulation of polysulfides in the transition between sulfur and lithium sulfide

Yongsheng Fu, Zhen Wu, Yifei Yuan, Peng Chen, Lei Yu, Lei Yuan, Qiurui Han, Yingjie Lan, Wuxin Bai, Erjun Kan, Chengxi Huang, Xiaoping Ouyang, Xin Wang, Junwu Zhu () and Jun Lu ()
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Yongsheng Fu: Nanjing University of Science and Technology
Zhen Wu: Nanjing University of Science and Technology
Yifei Yuan: Chemical Sciences and Engineering Division, Argonne National Laboratory
Peng Chen: Nanjing University of Science and Technology
Lei Yu: Nanjing University of Science and Technology
Lei Yuan: Nanjing University of Science and Technology
Qiurui Han: Nanjing University of Science and Technology
Yingjie Lan: Nanjing University of Science and Technology
Wuxin Bai: Nanjing University of Science and Technology
Erjun Kan: Nanjing University of Science and Technology
Chengxi Huang: Nanjing University of Science and Technology
Xiaoping Ouyang: Xiangtan University
Xin Wang: Nanjing University of Science and Technology
Junwu Zhu: Nanjing University of Science and Technology
Jun Lu: Chemical Sciences and Engineering Division, Argonne National Laboratory

Nature Communications, 2020, vol. 11, issue 1, 1-10

Abstract: Abstract Encapsulation strategies are widely used for alleviating dissolution and diffusion of polysulfides, but they experience nonrecoverable structural failure arising from the repetitive severe volume change during lithium−sulfur battery cycling. Here we report a methodology to construct an electrochemically recoverable protective layer of polysulfides using an electrolyte additive. The additive nitrogen-doped carbon dots maintain their “dissolved” status in the electrolyte at the full charge state, and some of them function as active sites for lithium sulfide growth at the full discharge state. When polysulfides are present amid the transition between sulfur and lithium sulfide, nitrogen-doped carbon dots become highly reactive with polysulfides to form a solid and recoverable polysulfide-encapsulating layer. This design skilfully avoids structural failure and efficiently suppresses polysulfide shuttling. The sulfur cathode delivers a high reversible capacity of 891 mAh g−1 at 0.5 C with 99.5% coulombic efficiency and cycling stability up to 1000 cycles at 2 C.

Date: 2020
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DOI: 10.1038/s41467-020-14686-2

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