Articles | Volume 5, issue 1
https://doi.org/10.5194/mr-5-87-2024
https://doi.org/10.5194/mr-5-87-2024
Research article
 | 
25 Jun 2024
Research article |  | 25 Jun 2024

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

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

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Cited articles

Armand, M. and Tarascon, J.: Building better batteries, Nature, 451, 2–7, 2008. a
Bhattacharyya, R., Key, B., Chen, H., Best, A. S., Hollenkamp, A. F., and Grey, C. P.: In situ NMR observation of the formation of metallic lithium microstructures in lithium batteries, Nat. Mater., 9, 504–510, https://doi.org/10.1038/nmat2764, 2010. a
Chandrashekar, S., Trease, N. M., Chang, H. J., Du, L.-S., Grey, C. P., and Jerschow, A.: Li MRI of Li batteries reveals location of microstructural lithium, Nat. Mater., 11, 311–315, https://doi.org/10.1038/nmat3246, 2012. a
Dutoit, C.-E.: Second harmonic EPR spectroscopy and imaging reveal Li-metal depositions in Li-ion batteries, Zenodo [data set], https://doi.org/10.5281/zenodo.10623150, 2024. a
Dutoit, C. E., Tang, M., Gourier, D., Tarascon, J. M., Vezin, H., and Salager, E.: Monitoring metallic sub-micrometric lithium structures in Li-ion batteries by in situ electron paramagnetic resonance correlated spectroscopy and imaging, Nat. Commun., 12, 1–6, https://doi.org/10.1038/s41467-021-21598-2, 2021. a, b, c
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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 (EPR) to identify traces of non-dendritic Li metal present on the graphite anode after multiple electrochemical cycles. Such metallic complexes are a source of limitations which reduce battery life and lead to serious safety issues. To improve their detection, we propose to simultaneously record the first- and second-harmonic EPR spectra.