Liquid-Based Janus Electrolyte for Sustainable Redox Mediation in Lithium–Oxygen Batteries

Youngmin Ko, Hong I. Kim, Sung Ju Cho, Kyung Min Lee, Gwan Yeong Jung, Hyeokjun Park, Se Hwan Park, Yun Jung Lee, Youngjoon Bae, Young Ro Lee, Kyoungoh Kim, Sang Kyu Kwak, Sang Young Lee, Kisuk Kang

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5 Citations (Scopus)


The discovery of a reliable electrolyte system remains one of the key challenges for the development of advanced lithium–oxygen batteries. To date, no single electrolyte is verified to be stable and compatible with both the cathode (e.g., oxygen radicals, lithium peroxide, etc.) and anode (lithium metal) for lithium–oxygen batteries. In this work, a novel liquid-based Janus electrolyte system consisting of two different immiscible liquid phases is proposed and it is demonstrated that this system is remarkably effective in promoting the sustainable operation of redox-mediated lithium–oxygen batteries. The liquid-based Janus electrolyte is rationally designed by considering its compatibility with the lithium–oxygen cell environment, the solubility difference of target soluble species, and the mutual immiscibility of the two liquid phases. By combining spectral characterization, a phase-separation experiment, and in situ observation of the electrochemical cell, it is revealed that the liquid-based Janus electrolyte suppresses the migration of redox mediators from one liquid phase to the other, thereby preventing the detrimental shuttle effect. The enhanced stability of redox mediation leads to improved cycling performance of the cell. The various combinations possible for the liquid-based Janus electrolyte open a new unexplored pathway for the design of advanced electrolyte systems for lithium–oxygen batteries.

Original languageEnglish
Article number2102096
JournalAdvanced Energy Materials
Issue number38
Publication statusPublished - 2021 Oct 14

Bibliographical note

Funding Information:
Y.K. and H.‐I.K. contributed equally to this work. This work was supported by the National Research Foundation of Korea(NRF) grant funded by the Korea government(MSIP) (NRF‐2017M1A2A2087812, NRF‐2018R1A2A1A05079249, NRF‐2019M3E6A1064522 and NRF‐2021R1A2B5B03001615). This research was supported by Creative Materials Discovery Program through the National Research Foundation of Korea (NRF) funded by the Ministry of Science, ICT and Future Planning (NRF‐2017M3D1A1039553). This work was also supported by Project Code. (IBS‐R006‐A2).

Publisher Copyright:
© 2021 Wiley-VCH GmbH

All Science Journal Classification (ASJC) codes

  • Renewable Energy, Sustainability and the Environment
  • Materials Science(all)


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