Advancing electrochemical impedance analysis through innovations in the distribution of relaxation times method

Adeleke Maradesa, Baptiste Py, Jake Huang, Yang Lu, Pietro Iurilli, Aleksander Mroziński, Ho Mei Law, Yuhao Wang, Zilong Wang, Jingwei Li, Shengjun Xu, Quentin Meyer, Jiapeng Liu, Claudio Brivio, Alexander Gavrilyuk, Kiyoshi Kobayashi, Antonio Bertei, Nicholas J. Williams, Chuan Zhao, Michael DanzerMark Žic, Phillip Wu, Ville Yrjänä, Sergei Pereverzyev, Yuhui Chen, André Weber, Sergei V. Kalinin, Jan Philipp Schmidt, Yoed Tsur, Bernard A. Boukamp, Qiang Zhang, Miran Gaberšček, Ryan O'Hayre, Francesco Ciucci*

*Corresponding author for this work

Research output: Contribution to journalReview Article or Literature Reviewpeer-review

124 Citations (Scopus)

Abstract

Electrochemical impedance spectroscopy (EIS) is widely used in electrochemistry, energy sciences, biology, and beyond. Analyzing EIS data is crucial, but it often poses challenges because of the numerous possible equivalent circuit models, the need for accurate analytical models, the difficulties of nonlinear regression, and the necessity of managing large datasets within a unified framework. To overcome these challenges, non-parametric models, such as the distribution of relaxation times (DRT, also known as the distribution function of relaxation times, DFRT), have emerged as promising tools for EIS analysis. For example, the DRT can be used to generate equivalent circuit models, initialize regression parameters, provide a time-domain representation of EIS spectra, and identify electrochemical processes. However, mastering the DRT method poses challenges as it requires mathematical and programming proficiency, which may extend beyond experimentalists’ usual expertise. Post-inversion analysis of DRT data can be difficult, especially in accurately identifying electrochemical processes, leading to results that may not always meet expectations. This article examines non-parametric EIS analysis methods, outlining their strengths and limitations from theoretical, computational, and end-user perspectives, and provides guidelines for their future development. Moreover, insights from survey data emphasize the need to develop a large impedance database, akin to an impedance genome. In turn, software development should target one-click, fully automated DRT analysis for multidimensional EIS spectra interpretation, software validation, and reliability. Particularly, creating a collaborative ecosystem hinged on free software could promote innovation and catalyze the adoption of the DRT method throughout all fields that use impedance data.
Original languageEnglish
Pages (from-to)1958-1981
Number of pages24
JournalJoule
Volume8
Issue number7
DOIs
Publication statusPublished - 17 Jul 2024
MoE publication typeA2 Review article in a scientific journal

Funding

A.M. B.P. and F.C. gratefully acknowledge the Research Grant Council of Hong Kong for support through projects 18201820 and 16201622. A.M. and B.P. kindly thank the Hong Kong PhD Fellowship Scheme for its financial support. F.C. thanks the University of Bayreuth and the Bavarian Center for Battery Technology (BayBatt) for providing a start-up fund. R.O. and J.H. acknowledge support from the Hydrogen in Energy and Information Sciences (HEISs) center, an Energy Frontier Research Center funded by the U.S. Department of Energy (DOE), Office of Science, Basic Energy Sciences (BES), under award no. DE-SC0023450 (DRT estimation methodology and software development), and by the Army Research Office (ARO) under Award 1305 no. W911NF-22-1-0273 (experimental application of EIS/DRT to electrochemical devices), and as part of the Energy Frontier Research Centers program: CSSAS-The Center for the Science of Synthesis Across Scales under award no. DE-SC0019288. A.M.: survey design, data collection, data curation, formal analysis, visualization, writing \u2013 review & editing, writing \u2013 original draft. B.P.: visualization, writing \u2013 review & editing. J.H.: visualization, writing \u2013 review & editing. Y.L.: writing \u2013 review & editing. P.I.: writing \u2013 review & editing. A.M.: writing \u2013 review & editing. H.M.L.: visualization, writing \u2013 review & editing. Y.W.: data collection, writing \u2013 review & editing. Z.W.: writing \u2013 review & editing. J. Li: writing \u2013 review & editing. S.X.: writing \u2013 review & editing. Q.M.: writing \u2013 review & editing. J. Liu: writing \u2013 review & editing. C.B.: supervision, writing \u2013 review & editing. A.G.: writing \u2013 review & editing. K.K.: writing \u2013 review & editing. A.B.: writing \u2013 review & editing. N.J.W.: writing \u2013 review & editing. C.Z.: supervision, writing \u2013 review & editing. M.D.: writing \u2013 review & editing. M.Z.: writing \u2013 review & editing. P.W.: writing \u2013 review & editing. V.Y.: writing \u2013 review & editing. S.P.: writing \u2013 review & editing. Y.C.: writing \u2013 review & editing. A.W.: writing \u2013 review & editing. S.V.K.: funding acquisition, writing \u2013 review & editing. J.P.S.: writing \u2013 review & editing. Y.T.: writing \u2013 review & editing. B.A.B.: writing \u2013 review & editing. Q.Z.: supervision, writing \u2013 review & editing. M.G.: writing \u2013 review & editing. R.O.: supervision, visualization, funding acquisition, writing \u2013 review & editing. F.C.: survey design, data collection, resources, project administration, funding acquisition, supervision, writing \u2013 review & editing, writing \u2013 original draft. The authors declare no competing interests. Upon editing the manuscript, the authors used Gemini Advanced to improve readability. After using this tool, the authors reviewed and re-edited the content as needed. The authors take full responsibility for the content of the published article. A.M., B.P., and F.C. gratefully acknowledge the Research Grant Council of Hong Kong for support through projects 18201820 and 16201622. A.M. and B.P. kindly thank the Hong Kong PhD Fellowship Scheme for its financial support. R.O. and J.H. acknowledge support from the Hydrogen in Energy and Information Sciences (HEISs) center, an Energy Frontier Research Center funded by the U.S. Department of Energy (DOE), Office of Science, Basic Energy Sciences (BES) , under award no. DE-SC0023450 (DRT estimation methodology and software development), and by the Army Research Office (ARO) under Award 1305 no. W911NF-22-1-0273 (experimental application of EIS/DRT to electrochemical devices), and as part of the Energy Frontier Research Centers program: CSSAS-The Center for the Science of Synthesis Across Scales under award no. DE-SC0019288 .

Keywords

  • distribution of relaxation times
  • electrochemical impedance spectroscopy
  • methods development
  • inverse problems
  • electrochemical systems

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