Open AccessFingerprinting Redox Heterogeneity in Electrodes during Extreme Fast Charging
Author(s) -
Aashutosh Mistry,
François Usseglio-Viretta,
Andrew M. Colclasure,
Kandler Smith,
Partha P. Mukherjee
Publication year - 2020
Publication title -
journal of the electrochemical society
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 1.258
H-Index - 271
eISSN - 1945-7111
pISSN - 0013-4651
DOI - 10.1149/1945-7111/ab8fd7
Subject(s) - electrode , anode , cathode , electrochemistry , lithium (medication) , chemical physics , homogeneous , battery (electricity) , materials science , redox , scaling , range (aeronautics) , observability , chemistry , physics , statistical physics , thermodynamics , composite material , medicine , power (physics) , geometry , mathematics , metallurgy , endocrinology
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.