Volume 79
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Jiang, F.-N., Yang, S.-J., Chen, Z.-X., Liu, H., Yuan, H., Liu, L., . . . Zhang, Q. (2023). Higher-order polysulfides induced thermal runaway for 1.0 Ah lithium sulfur pouch cells. Particuology, 79, 10-17. https://doi.org/10.1016/j.partic.2022.11.009
Higher-order polysulfides induced thermal runaway for 1.0 Ah lithium sulfur pouch cells (Open Access)
Feng-Ni Jiang a b, Shi-Jie Yang c, Zi-Xian Chen c, He Liu c e, Hong Yuan c, Lei Liu a, Jia-Qi Huang c, Xin-Bing Cheng d, Qiang Zhang b
a College of Chemical Engineering and Technology, Taiyuan University of Technology, Taiyuan, 030024, Shanxi, China
b Beijing Key Laboratory of Green Chemical Reaction Engineering and Technology, Department of Chemical Engineering, Tsinghua University, Beijing, 100084, China
c Advanced Research Institute of Multidisciplinary Science, Beijing Institute of Technology, Beijing, 100081, China
d Key Laboratory of Energy Thermal Conversion and Control of Ministry of Education, School of Energy and Environment, Southeast University, Nanjing, 211189, Jiangsu, China
e School of Chemistry and Materials Science, Nanjing University of Information Science and Technology, Nanjing, 210044, Jiangsu, China
10.1016/j.partic.2022.11.009
Volume 79, August 2023, Pages 10-17
Received 17 October 2022, Revised 17 November 2022, Accepted 20 November 2022, Available online 8 December 2022, Version of Record 24 January 2023.
E-mail: chengxb@seu.edu.cn

Highlights

• The thermal safety of deeply cycled Li–S pouch cells have been systematically investigated.

• Thermal behaviors of 16-cycle cells with/without electrolytes are due to different viscosities.

• The thermal safety of 16/45-cycle cells depends on the polysulfides species in electrolytes.


Abstract

Comprehensive analyses on thermal runaway mechanisms are critically vital to achieve the safe lithium–sulfur (Li–S) batteries. The reactions between dissolved higher-order polysulfides and Li metal were found to be the origins for the thermal runaway of 1.0 Ah cycled Li–S pouch cells. 16-cycle pouch cell indicates high safety, heating from 30 to 300 °C without thermal runaway, while 16-cycle pouch cell with additional electrolyte undergoes severe thermal runaway at 147.9 °C, demonstrating the key roles of the electrolyte on the thermal safety of batteries. On the contrary, thermal runaway does not occur for 45-cycle pouch cell despite the addition of the electrolyte. It is found that the higher-order polysulfides (Li2Sx ≥ 6) are discovered in 16-cycle electrolyte while the sulfur species in 45-cycle electrolyte are Li2Sx ≤ 4. In addition, strong exothermic reactions are discovered between cycled Li and dissolved higher-order polysulfide (Li2S6 and Li2S8) at 153.0 °C, driving the thermal runaway of cycled Li–S pouch cells. This work uncovers the potential safety risks of Li–S batteries and negative roles of the polysulfide shuttle for Li–S batteries from the safety view.

Graphical abstract
Keywords
Lithium–sulfur batteries; Thermal runaway; Polysulfides; Pouch cell; Polysulfide shuttle