Preprints
https://doi.org/10.5194/mr-2024-5
https://doi.org/10.5194/mr-2024-5
18 Mar 2024
 | 18 Mar 2024
Status: this preprint is currently under review for the journal MR.

Second harmonic electron paramagnetic resonance spectroscopy and imaging reveal metallic lithium depositions in Li-ion batteries

Charles-Emmanuel Dutoit, Hania Ahouari, Quentin Denoyelle, Simon Pondaven, and Hervé Vezin

Abstract. We have investigated the metallic lithium particles nucleation following lithiation and delithiation steps of the graphite electrode using X-band electron paramagnetic resonance (EPR). Metallic lithium aggregates like dendrites and/or filaments which are formed during electrochemical cycling on the graphite anode are complex structures which may lead to internal short-circuit and safety issues. Understanding and following, in real conditions, this nucleation process is necessary to improve the development of Li-ion batteries. The complexity to detect metallic lithium structures inside Li-ion batteries depends on the number of EPR lines and their linewidth. The presence of lithiated graphite phases affects the detection of micrometric Li-metal elements. Herein, we report a new approach using cw-EPR spectroscopy and imaging combining the first and the second harmonic detection schemes to provide evidence of the metallic lithium aggregates nucleation in these negative electrodes. Although the first harmonic gives all the EPR signals present in the sample, it is found that the second harmonic EPR signal is mainly sensitive to metallic lithium depositions.

Charles-Emmanuel Dutoit, Hania Ahouari, Quentin Denoyelle, Simon Pondaven, and Hervé Vezin

Status: open (until 02 May 2024)

Comment types: AC – author | RC – referee | CC – community | EC – editor | CEC – chief editor | : Report abuse
  • RC1: 'Comment on mr-2024-5', Hu Bingwen, 28 Mar 2024 reply
    • AC1: 'Reply on RC1', Charles Dutoit, 03 Apr 2024 reply
      • RC2: 'Reply on AC1', Hu Bingwen, 10 Apr 2024 reply
        • AC2: 'Reply on RC2', Charles Dutoit, 12 Apr 2024 reply
          • RC3: 'Reply on AC2', Hu Bingwen, 16 Apr 2024 reply
            • AC3: 'Reply on RC3', Charles Dutoit, 16 Apr 2024 reply
              • RC4: 'Reply on AC3', Hu Bingwen, 16 Apr 2024 reply
              • RC5: 'Reply on AC3', Hu Bingwen, 16 Apr 2024 reply
              • RC6: 'Reply on AC3', Hu Bingwen, 16 Apr 2024 reply
              • RC7: 'Reply on AC3', Hu Bingwen, 16 Apr 2024 reply
Charles-Emmanuel Dutoit, Hania Ahouari, Quentin Denoyelle, Simon Pondaven, and Hervé Vezin
Charles-Emmanuel Dutoit, Hania Ahouari, Quentin Denoyelle, Simon Pondaven, and Hervé Vezin

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Short summary
In our study, we correlate the first and the second harmonic detection modes of continuous wave electron paramagnetic resonance to identify metallic lithium traces present on the graphite anode after multi electrochemical cycles. Such metallic complexes are a source of limitations which reduces battery life and lead to serious safety issues. To improve their detection, we propose to record simultaneously the first and the second harmonic EPR spectrum.