A versatile functionalized ionic liquid to boost the solution-mediated performances of lithium-oxygen batteries

Jinqiang Zhang, Bing Sun, Yufei Zhao, Anastasia Tkacheva, Zhenjie Liu, Kang Yan, Xin Guo, Andrew M. McDonagh, Devaraj Shanmukaraj, Chengyin Wang, Teofilo Rojo, Michel Armand (), Zhangquan Peng () and Guoxiu Wang ()
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Jinqiang Zhang: University of Technology Sydney, Broadway
Bing Sun: University of Technology Sydney, Broadway
Yufei Zhao: University of Technology Sydney, Broadway
Anastasia Tkacheva: University of Technology Sydney, Broadway
Zhenjie Liu: Chinese Academy of Sciences
Kang Yan: University of Technology Sydney, Broadway
Xin Guo: University of Technology Sydney, Broadway
Andrew M. McDonagh: University of Technology Sydney, Broadway
Devaraj Shanmukaraj: CIC EnergiGUNE
Chengyin Wang: Yangzhou University
Teofilo Rojo: CIC EnergiGUNE
Michel Armand: CIC EnergiGUNE
Zhangquan Peng: Chinese Academy of Sciences
Guoxiu Wang: University of Technology Sydney, Broadway

Nature Communications, 2019, vol. 10, issue 1, 1-10

Abstract: Abstract Due to the high theoretical specific energy, the lithium–oxygen battery has been heralded as a promising energy storage system for applications such as electric vehicles. However, its large over-potentials during discharge–charge cycling lead to the formation of side-products, and short cycle life. Herein, we report an ionic liquid bearing the redox active 2,2,6,6-tetramethyl-1-piperidinyloxy moiety, which serves multiple functions as redox mediator, oxygen shuttle, lithium anode protector, as well as electrolyte solvent. The additive contributes a 33-fold increase of the discharge capacity in comparison to a pure ether-based electrolyte and lowers the over-potential to an exceptionally low value of 0.9 V. Meanwhile, its molecule facilitates smooth lithium plating/stripping, and promotes the formation of a stable solid electrolyte interface to suppress side-reactions. Moreover, the proportion of ionic liquid in the electrolyte influences the reaction mechanism, and a high proportion leads to the formation of amorphous lithium peroxide and a long cycling life (> 200 cycles). In particular, it enables an outstanding electrochemical performance when operated in air.

Date: 2019
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DOI: 10.1038/s41467-019-08422-8

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