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Fingerprinting Redox Heterogeneity in Electrodes during Extreme Fast Charging

preprint
submitted on 02.12.2019 and posted on 11.12.2019 by Aashutosh Mistry, Francois L. E. Usseglio-Viretta, Andrew Colclasure, Kandler Smith, Partha P. Mukherjee
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 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.

History

Email Address of Submitting Author

amistry@anl.gov

Institution

Argonne National Laboratory

Country

USA

ORCID For Submitting Author

0000-0002-4359-4975

Declaration of Conflict of Interest

No conflict of interest

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