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Singlet oxygen generation as a major cause for parasitic reactions during cycling of aprotic lithium–oxygen batteries

Author

Listed:
  • Nika Mahne

    (Institute for Chemistry and Technology of Materials, Graz University of Technology)

  • Bettina Schafzahl

    (Institute for Chemistry and Technology of Materials, Graz University of Technology)

  • Christian Leypold

    (Institute for Chemistry and Technology of Materials, Graz University of Technology)

  • Mario Leypold

    (Institute of Organic Chemistry, Graz University of Technology)

  • Sandra Grumm

    (Institute for Chemistry and Technology of Materials, Graz University of Technology)

  • Anita Leitgeb

    (Institute for Chemistry and Technology of Materials, Graz University of Technology)

  • Gernot A. Strohmeier

    (Institute of Organic Chemistry, Graz University of Technology
    Austrian Centre of Industrial Biotechnology (acib) GmbH)

  • Martin Wilkening

    (Institute for Chemistry and Technology of Materials, Graz University of Technology)

  • Olivier Fontaine

    (Institut Charles Gerhardt Montpellier
    Réseau sur le Stockage Électrochimique de l’Énergie (RS2E), CNRS FR3459, 33 rue Saint Leu)

  • Denis Kramer

    (Engineering Sciences, University Road, University of Southampton)

  • Christian Slugovc

    (Institute for Chemistry and Technology of Materials, Graz University of Technology)

  • Sergey M. Borisov

    (Institute for Analytical Chemistry and Food Chemistry, Graz University of Technology)

  • Stefan A. Freunberger

    (Institute for Chemistry and Technology of Materials, Graz University of Technology)

Abstract

Non-aqueous metal–oxygen batteries depend critically on the reversible formation/decomposition of metal oxides on cycling. Irreversible parasitic reactions cause poor rechargeability, efficiency, and cycle life, and have predominantly been ascribed to the reactivity of reduced oxygen species with cell components. These species, however, cannot fully explain the side reactions. Here we show that singlet oxygen forms at the cathode of a lithium–oxygen cell during discharge and from the onset of charge, and accounts for the majority of parasitic reaction products. The amount increases during discharge, early stages of charge, and charging at higher voltages, and is enhanced by the presence of trace water. Superoxide and peroxide appear to be involved in singlet oxygen generation. Singlet oxygen traps and quenchers can reduce parasitic reactions effectively. Awareness of the highly reactive singlet oxygen in non-aqueous metal–oxygen batteries gives a rationale for future research towards achieving highly reversible cell operation.

Suggested Citation

  • Nika Mahne & Bettina Schafzahl & Christian Leypold & Mario Leypold & Sandra Grumm & Anita Leitgeb & Gernot A. Strohmeier & Martin Wilkening & Olivier Fontaine & Denis Kramer & Christian Slugovc & Serg, 2017. "Singlet oxygen generation as a major cause for parasitic reactions during cycling of aprotic lithium–oxygen batteries," Nature Energy, Nature, vol. 2(5), pages 1-9, May.
    • Handle: RePEc:nat:natene:v:2:y:2017:i:5:d:10.1038_nenergy.2017.36
    DOI: 10.1038/nenergy.2017.36
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    Cited by:

    1. Deqing Cao & Chuan Tan & Yuhui Chen, 2022. "Oxidative decomposition mechanisms of lithium carbonate on carbon substrates in lithium battery chemistries," Nature Communications, Nature, vol. 13(1), pages 1-12, December.
    2. Liangbo Xie & Pengfei Wang & Yi Li & Dongpeng Zhang & Denghui Shang & Wenwen Zheng & Yuguo Xia & Sihui Zhan & Wenping Hu, 2022. "Pauling-type adsorption of O2 induced electrocatalytic singlet oxygen production on N–CuO for organic pollutants degradation," Nature Communications, Nature, vol. 13(1), pages 1-11, December.
    3. Chao-Hai Gu & Song Wang & Ai-Yong Zhang & Chang Liu & Jun Jiang & Han-Qing Yu, 2024. "Tuning electronic structure of metal-free dual-site catalyst enables exclusive singlet oxygen production and in-situ utilization," Nature Communications, Nature, vol. 15(1), pages 1-11, December.

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