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Assessing cathode–electrolyte interphases in batteries

Nature Energy volume 9, pages 1463–1473 (2024)Cite this article

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Abstract

The cathode–electrolyte interphase plays a pivotal role in determining the usable capacity and cycling stability of electrochemical cells, yet it is overshadowed by its counterpart, the solid–electrolyte interphase. This is primarily due to the prevalence of side reactions, particularly at low potentials on the negative electrode, especially in state-of-the-art Li-ion batteries where the charge cutoff voltage is limited. However, as the quest for high-energy battery technologies intensifies, there is a pressing need to advance the study of cathode–electrolyte interphase properties. Here, we present a comprehensive approach to analyse the cathode–electrolyte interphase in battery systems. We underscore the importance of employing model cathode materials and coin cell protocols to establish baseline performance. Additionally, we delve into the factors behind the inconsistent and occasionally controversial findings related to the cathode–electrolyte interphase. We also address the challenges and opportunities in characterizing and simulating the cathode–electrolyte interphase, offering potential solutions to enhance its relevance to real-world applications.

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Fig. 1: Single-crystal Ni-rich NMC with different morphologies as model materials.
Fig. 2: Electrochemical performance of NMC811 polycrystals tested in full coin cells that use graphite as anode.
Fig. 3: Electrical double layers formed on positive electrode (cathode in battery) and negative electrode sides (anode in battery) during charge process.
Fig. 4: An approach for resolving the chemical and structural features of complex electrochemical interphases on the basis of the integration of experiments and theory.

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Acknowledgements

This work was supported by the Assistant Secretary for Energy Efficiency and Renewable Energy, Office of Vehicle Technologies of the US Department of Energy (DOE) through the Cathode–Electrolyte Interphase (CEI) Consortium. Pacific Northwest National Laboratory (PNNL) is operated by Battelle for the DOE under contract DE-AC05-76RL01830. Part of the work was performed under the auspices of the US DOE by Lawrence Livermore National Laboratory under contract DEAC52-07NA27344. Sandia National Laboratories is a multi-mission laboratory managed and operated by National Technology and Engineering Solutions of Sandia LLC, a wholly-owned subsidiary of Honeywell International Inc., for the US DOE’s National Nuclear Security Administration under contract DE-NA-0003525.

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Authors and Affiliations

  1. Pacific Northwest National Laboratory, Richland, WA, USA

    Jie Xiao, Yujing Bi, Jun Liu, Chongmin Wang, Bingbin Wu & Yaobin Xu

  2. University of Washington, Seattle, WA, USA

    Jie Xiao, Corie L. Cobb & Jun Liu

  3. San Francisco State University, San Francisco, CA, USA

    Nicole Adelstein

  4. Idaho National Laboratory, Idaho Falls, ID, USA

    Wenjuan Bian

  5. Argonne National Laboratory, Lemont, IL, USA

    Jordi Cabana

  6. SLAC National Accelerator Laboratory, Menlo Park, CA, USA

    Yi Cui

  7. Stanford University, Stanford, CA, USA

    Yi Cui

  8. University of California Irvine, Irvine, CA, USA

    Shen J. Dillon

  9. Lawrence Berkeley National Laboratory, Berkeley, CA, USA

    Marca M. Doeff & Wei Tong

  10. Jackson State University, Jackson, MS, USA

    Saiful M. Islam

  11. Sandia National Laboratories, Albuquerque, NM, USA

    Kevin Leung

  12. Oak Ridge National Laboratory, Oak Ridge, TN, USA

    Mengya Li & Ritu Sahore

  13. Virginia Tech, Blacksburg, VA, USA

    Feng Lin

  14. New Mexico State University, Las Cruces, NM, USA

    Hongmei Luo

  15. Brookhaven National Laboratory, Upton, NY, USA

    Amy C. Marschilok

  16. Stony Brook University, Stony Brook, NY, USA

    Amy C. Marschilok

  17. University of Chicago, Chicago, IL, USA

    Ying Shirley Meng

  18. Brown University, Providence, RI, USA

    Yue Qi

  19. University of Colorado Boulder, Boulder, CO, USA

    Kayla G. Sprenger & Michael F. Toney

  20. National Renewable Energy Laboratory, Golden, CO, USA

    Robert C. Tenent

  21. Lawrence Livermore National Laboratory, Livermore, CA, USA

    Liwen F. Wan & Stephen E. Weitzner

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Correspondence to Jie Xiao.

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Nature Energy thanks Yang-Kook Sun and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.

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Xiao, J., Adelstein, N., Bi, Y. et al. Assessing cathode–electrolyte interphases in batteries. Nat Energy 9, 1463–1473 (2024). https://doi.org/10.1038/s41560-024-01639-y

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