Fingerprinting Redox Heterogeneity in Electrodes during Extreme Fast Charging

Aashutosh Mistry, Francois Usseglio-Viretta, Andrew Colclasure, Kandler Smith, Partha Mukherjee

Research output: Contribution to journalArticlepeer-review

66 Scopus Citations


Conventionally, battery electrodes are rationalized as homogeneous reactors. It proves to be an erroneous interpretation for fast transients, where mass transport limitations amplify underlying heterogeneities. Given the lack of observability of associated fast spatiotemporal dynamics, redox activity in inhomogeneous electrodes is superficially explored. We resort to a physics-based description to examine the extreme fast charging of lithium-ion battery electrodes. Representative inhomogeneity information is extracted from electrode tomograms. We discover such electrodes to undergo preferential intercalation, localized lithium plating and nonuniform heat generation as a result of distributed long- and short-range interactions. The spatial correlations of these events with the underlying inhomogeneity are found to be nonidentical. Investigation of multiple inhomogeneity fields reveals an exponential scaling of plating severity and early onset in contrast to the homogeneous limit. Anode and cathode inhomogeneities couple nonlinearly to grow peculiar electrodeposition patterns. These mechanistic insights annotate the complex functioning of spatially nonuniform electrodes.

Original languageAmerican English
Article number090542
Number of pages11
JournalJournal of the Electrochemical Society
Issue number9
StatePublished - 2020

Bibliographical note

Publisher Copyright:
© 2020 The Author(s). Published on behalf of The Electrochemical Society by IOP Publishing Limited.

NREL Publication Number

  • NREL/JA-5400-77255


  • fast charging batteries
  • lithium-ion batteries
  • redox reactions


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