Article

Electrochemical stiffness in lithium-ion batteries

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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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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.

Author information

Author notes

    • Hadi Tavassol
    •  & Elizabeth M. C. Jones

    These authors contributed equally to this work.

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

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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.

Competing interests

The authors declare no competing financial interests.

Corresponding authors

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

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