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Electrochemical stiffness in lithium-ion batteries

Nature Materials volume 15, pages 1182–1187 (2016)Cite this article

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Abstract

Although lithium-ion batteries are ubiquitous in portable electronics, increased charge rate and discharge power are required for more demanding applications such as electric vehicles. The high-rate exchange of lithium ions required for more power and faster charging generates significant stresses and strains in the electrodes that ultimately lead to performance degradation. To date, electrochemically induced stresses and strains in battery electrodes have been studied only individually. Here, a new technique is developed to probe the chemomechanical response of electrodes by calculating the electrochemical stiffness via coordinated in situ stress and strain measurements. We show that dramatic changes in electrochemical stiffness occur due to the formation of different graphite–lithium intercalation compounds during cycling. Our analysis reveals that stress scales proportionally with the lithiation/delithiation rate and strain scales proportionally with capacity (and inversely with rate). Electrochemical stiffness measurements provide new insights into the origin of rate-dependent chemomechanical degradation and the evaluation of advanced battery electrodes.

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Figure 1: Methodology for electrochemical stiffness calculations.
Figure 2: Potential-dependent electrode response during cyclic voltammetry.
Figure 3: Coordination of stress and strain measurements and calculation of the electrochemical stiffness.
Figure 4: Asynchronous development of stress and strain.
Figure 5: Effect of the potential scan rate on the development of stress and strain in graphite electrodes.

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Acknowledgements

This work was supported by the Center for Electrochemical Energy Science, an Energy Frontier Research Center funded by the US Department of Energy, Office of Science, Basic Energy Sciences. E.M.C.J. acknowledges graduate fellowships through the National Science Foundation and the Beckman Institute for Advanced Science and Technology. The authors thank J. Lyding for use of spot welding equipment.

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Author notes

  1. Hadi Tavassol and Elizabeth M. C. Jones: These authors contributed equally to this work.

Authors and Affiliations

  1. Department of Chemistry, University of Illinois at Urbana-Champaign, Urbana, Illinois 61801, USA

    Hadi Tavassol & Andrew A. Gewirth

  2. Department of Mechanical Science and Engineering, University of Illinois at Urbana-Champaign, Urbana, Illinois 61801, USA

    Elizabeth M. C. Jones

  3. Beckman Institute of Science and Technology, University of Illinois at Urbana-Champaign, Urbana, Illinois 61801, USA

    Elizabeth M. C. Jones & Nancy R. Sottos

  4. Department of Material Science and Engineering, University of Illinois at Urbana-Champaign, Urbana, Illinois 61801, USA

    Nancy R. Sottos

Authors
  1. Hadi Tavassol
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Contributions

The manuscript was written through contributions of all authors. H.T. performed all stress measurements, E.M.C.J. performed all strain measurements and electrochemical stiffness calculations, and H.T. and E.M.C.J. jointly performed all data analysis. All authors contributed to interpretation of the data, and all authors have given approval to the final version of the manuscript.

Corresponding authors

Correspondence to Nancy R. Sottos or Andrew A. Gewirth.

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The authors declare no competing financial interests.

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Tavassol, H., Jones, E., Sottos, N. et al. Electrochemical stiffness in lithium-ion batteries. Nature Mater 15, 1182–1187 (2016). https://doi.org/10.1038/nmat4708

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