For citation:
Kolosnitsyn D. V., Egorova N. V., Khasanova R. V., Kuzmina E. V., Karaseva E. V., Kolosnitsyn V. S. Differentiation of electrode contributions to the total impedance of lithium-sulfur cells using the distribution function of relaxation times. Electrochemical Energetics, 2026, vol. 26, iss. 1, pp. 13-28. DOI: 10.18500/1608-4039-2026-26-1-13-28, EDN: NKNFTQ
Differentiation of electrode contributions to the total impedance of lithium-sulfur cells using the distribution function of relaxation times
The analysis of electrochemical impedance of lithium-sulfur cells is complicated by the complexity of the processes occurring inside them. Both electrochemical processes and mass transport processes simultaneously occur on the lithium and sulfur electrodes of the cells, as well as in the bulk electrolyte. A comparative analysis of the distribution functions of relaxation times of symmetric Li||Li, S||Sand and the full lithium-sulfur cell has been conducted. Being a model-independent approach, the distribution functions of relaxation times method lets us objectively identify the number of relaxation processes and their relaxation times. The subsequent comparison of the data from the full and the symmetrical cells enables us to make a physically reasonable correlation of peaks on the distribution functions of relaxation times to specific electrodes.
- Chen Z. X., Hou L. P., Bi C. X., Cheng Q., Zhang X. Q., Li B. Q., Huang J. Q. Failure analysis of high-energy-density lithium–sulfur pouch cells. Energy Storage Materials, 2022, vol. 53, pp. 315–321 https://doi.org/10.1016/j.ensm.2022.07.035
- Privaldos O. L. A., Lee C., Kim J. W., Lee J. Exploring failure mechanism studies for lithium-sulfur battery pouch cells. Current Opinion in Electrochemistry, 2024, vol. 45, art. 101516 https://doi.org/10.1016/j.coelec.2024.101516
- Stojnov Z. B., Grafov B. M., SavovaStojnova B., Elkin V. V. Elektrokhimicheskij impedans [Electrochemical impedance]. Moscow, Nauka, 1991. 336 p. (in Russian).
- Ivanishchev A. V., Churikov A. V., Ivanishcheva I. A. Impedance spectroscopy of lithiumcarbon electrodes. Elektrokhimiya [Electrochemistry], 2009, vol. 44, no. 5, pp. 553–568 (in Russian).
- Kolosnitsyn V. S., Kuzmina E. V., Karaseva E. V., Mochalov S. E. A study of the electrochemical processes in lithium–sulphur cells by impedance spectroscopy. J. Power Sources, 2011, vol. 196, pp. 1478–1482. https://doi.org/10.1016/j.jpowsour.2010. 08.105
- Raccichini R., Amores M., Hinds G. Critical Review of the Use of Reference Electrodes in Li-Ion Batteries: A Diagnostic Perspective. Batteries, 2019, vol. 5, art. 12. https://doi.org/10.3390/batteries5010012
- Waluś S., Barchasz C., Bouchet R., Alloin F. Electrochemical impedance spectroscopy study of lithium–sulfur batteries: Useful technique to reveal the Li/S electrochemical mechanism. Electrochimica Acta, 2020, vol. 359, art. 136944. https://doi.org/10.1016/j.electacta.2020.136944
- Gavriliuk A. L., Osinkin D. A., Bronin D. I. On the application of Tikhonov’s regularization method to the calculation of the relaxation time distribution function in impedance spectroscopy. Elektrokhimiya [Electrochemistry], 2017, vol. 53, no. 6, pp. 651–655 (in Russian).
- Wan T. H., Saccoccio M., Chen C., Ciucci F. Influence of the Discretization Methods on the Distribution of Relaxation Times Deconvolution: Implementing Radial Basis Functions with DRTtools. Electrochimica Acta, 2015, vol. 184, pp. 483–499.
- Kolosnitsyn D. V. Program for computer “ElChemLab, DRTAnalyzer”, certificate 2022665869 RF. Owner Ufa Federal Research Centre of the Russian Academy of Sciences (RU). Published 23 August, 2022. 1 p.
- EC-Lab Software. Available at: https://www.biologic.net/softwares/ec-lab-software/ (accessed December 1, 2025).
- Aurbach D., Daroux M., McDougall G., Yeager E. B. Spectroscopic studies of lithium in an ultrahigh vacuum system. J. Electroanal. Chem., 1993, vol. 358, pp. 63–76. https://doi.org/10.1016/0022- 0728(93)80431-G
- Zaban A., Zinigrad E., Aurbach D. Impedance Spectroscopy of Li Electrodes. 4. A General Simple Model of the Li-Solution Interphase in Polar Aprotic Systems, J. Phys. Chem., 1996, vol. 100, pp. 3089– 3101.
- Kolosnitsyn D. V., Osipova D. A., Kuzmina E. V., Karaseva E. V., Kolosnitsyn V. S. Analysis of Impedance Spectra of a Lithium Electrode by the Distribution of Relaxation Times. Russian Journal of Electrochemistry, 2023, vol. 59, no. 7, p. 524–537. https://doi.org/10.1134/s1023193523070054
- Chen X., Li L., Liu M., Huang T., Yu A. Detection of lithium plating in lithium-ion batteries by distribution of relaxation times. J. Power Sources, 2021, vol. 496, art. 229867.