Asphericity Can Cause Nonuniform Lithium Intercalation in Battery Active Particles

Aashutosh Mistry, Thomas Heenan, Kandler Smith, Paul Shearing, Partha Mukherjee

Research output: Contribution to journalArticlepeer-review

19 Scopus Citations


Uniform intercalation is desired to enable next-generation Li-ion batteries. While we expect nonuniformity in materials undergoing a phase change, single-phase intercalation materials such as nickel manganese cobalt oxide are believed to lithiate uniformly at the particle/electrolyte interface. However, recent imaging reveals nonuniform lithiation. Motivated by this discrepancy, we examine if aspherical particle shape can cause such nonuniformity since the conventional belief is based on spherical particle theory. We obtain real particle geometries using rapid lab-based X-ray computed tomography and subsequently perform physics-based calculations accounting for electrochemical reactions at the particle/electrolyte interface and lithium transport inside the particle bulk. The aspherical geometry breaks the symmetry and causes nonuniform reaction distribution. Such nonuniformity is exacerbated as the particle becomes more aspherical. The proposed mechanism represents a fundamental limit on achievable lithiation uniformity in aspherical particles in the absence of other mechanisms causing inhomogeneity, such as grain structure, nonuniform carbon-binder coating, etc.

Original languageAmerican English
Pages (from-to)1871-1879
Number of pages9
JournalACS Energy Letters
Issue number5
StatePublished - 2022

Bibliographical note

Publisher Copyright:
© 2022 UChicago Argonne, LLC, Operator of Argonne National Laboratory. Published by American Chemical Society.

NREL Publication Number

  • NREL/JA-5700-82974


  • aspherical particle shape
  • Li-ion batteries
  • lithiation
  • nonuniformity
  • single-phase intercalation materials


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