Columnar order in jammed LiFePO 4 cathodes: Ion transport catastrophe and its mitigation

Kyle C. Smith, Partha P. Mukherjee, Timothy S. Fisher

Research output: Contribution to journalArticlepeer-review


The high-rate, high-capacity potential of LiFePO 4-based lithium-ion battery cathodes has motivated numerous experimental and theoretical studies aiming to realize such performance through nano-sizing, tailoring of particle shape through synthesis conditions, and doping. Here, a granular mechanics study of microstructures formed by dense jammed packings of experimentally and theoretically inspired LiFePO 4 particle shapes is presented. A strong dependence of the resultant packing structures on particle shapes is observed, in which columnar structures aligned with the [010] direction inhibit diffusion along [010] in anisotropic LiFePO 4. Transport limitations are induced by [010] columnar order and lead to catastrophic performance degradation in anisotropic LiFePO 4 electrodes. Further, judicious mixing of nanoplatelets with additive nanoparticles can frustrate columnar ordering and thereby enhance the rate capability of LiFePO 4 electrodes by nearly an order of magnitude.

Original languageEnglish (US)
Pages (from-to)7040-7050
Number of pages11
JournalPhysical Chemistry Chemical Physics
Issue number19
StatePublished - May 21 2012
Externally publishedYes

ASJC Scopus subject areas

  • General Physics and Astronomy
  • Physical and Theoretical Chemistry


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