Asphericity Can Cause Nonuniform Lithium Intercalation in Battery Active Particles

Mistry, Aashutosh; Heenan, Thomas; Smith, Kandler; Shearing, Paul; Mukherjee, Partha P.

doi:10.1021/acsenergylett.2c00870

Title: Asphericity Can Cause Nonuniform Lithium Intercalation in Battery Active Particles

Journal Article · 05 May 2022 · ACS Energy Letters

DOI:https://doi.org/10.1021/acsenergylett.2c00870· OSTI ID:1869280

Mistry, Aashutosh; Heenan, Thomas;

; Shearing, Paul; Mukherjee, Partha P.

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.

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Research Organization:: National Renewable Energy Lab. (NREL), Golden, CO (United States)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V), eXtreme Fast Charge and Cell Evaluation of Lithium-Ion Batteries (XCEL) Program

DOE Contract Number:: AC36-08GO28308

OSTI ID:: 1869280

Report Number(s):: NREL/JA-5700-82974; MainId:83747; UUID:9bb034c9-5d2c-43fe-9cb3-25fe7daba29b; MainAdminID:64543

Journal Information:: ACS Energy Letters, Vol. 7, Issue 5

Country of Publication:: United States

Language:: English

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