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Redox mediators (RMs) suppress the charging overpotential to enhance the cycle performance of lithium-air batteries (LABs), but inappropriate RM incorporation can adversely shorten the cycle life. In this study, three typical organic RMs of tetrathiafulvalene (TTF), 2,2,6,6-tetramethylpiperidine 1-oxyl (TEMPO), and 10-methylphenothiazine (MPT) were incorporated into the air-electrode of LAB (RM-on-AE), rather than dissolving them in the electrolyte (RM-in-EL), to maximize the RM effect throughout the cycle life. The discharge/charge cycle test clarified that the cells with RM-on-AE prevented the reductive decomposition of RM with lithium anode, deriving the RM effect for longer cycle life than the cells with RM-in-EL. The quantification of AE deposits revealed that the TTF- and TEMPO-on-AE cells hardly generated a quantitative amount of Li2O2 discharge product, while the MPT-on-AE provided 96% yield of Li2O2 after discharge. The quantitative analysis also revealed an accumulation of Li2CO3 on the AEs, along with the generation of carboxylate. Because this was also true for the MPT-on-AE cells, further improvement of oxidative tolerance is needed for the substantial increase on the battery cycle life. This study provides appropriate RM introduction for the development of long-life LABs.

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• Creative Commons BY-NC-ND Attribution-NonCommercial-NoDerivs 4.0 International
  

  This is the Accepted Manuscript version of an article accepted for publication in Journal of The Electrochemical Society. IOP Publishing Ltd is not responsible for any errors or omissions in this version of the manuscript or any version derived from it. The Version of Record is available online at https://doi.org/10.1149/1945-7111/ad7f92.

Keyword: redox-mediator, lithium-air, battery, air-electrode

Date published: 2024-10-01

Publisher: The Electrochemical Society

Journal:

• Journal of The Electrochemical Society (ISSN: 00134651) vol. 171 issue. 10 100511

Funding:

• Advanced Low Carbon Technology Research and Development Program JPMJAL1301

Manuscript type: Author's version (Accepted manuscript)

MDR DOI: https://doi.org/10.48505/nims.4833

First published URL: https://doi.org/10.1149/1945-7111/ad7f92

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Updated at: 2025-10-21 15:50:56 +0900

Published on MDR: 2025-10-21 15:43:09 +0900