Multiscale dynamics of charging and plating in graphite electrodes coupling operando microscopy and phase-field modelling
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s41467-023-40574-6.pdf
Description
Published version
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7.01 MB
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Checksum (MD5)
cbc0dc565d4b5ba50c968457edd2ea09
Author(s)
Lu, Xuekun
Lagnoni, Marco
Bertei, Antonio
Das, Supratim
Owen, Rhodri E
Li, Qi
O’Regan, Kieran
Wade, Aaron
Finegan, Donal P
Kendrick, Emma
Date Issued
2023
Journal
Nature Communications
Publisher
Springer Science and Business Media LLC
Citation
Lu, X., Lagnoni, M., Bertei, A. et al. Multiscale dynamics of charging and plating in graphite electrodes coupling operando microscopy and phase-field modelling. Nat Commun 14, 5127 (2023).
Version
Final published version
Abstract
The phase separation dynamics in graphitic anodes significantly affects lithium plating propensity, which is the major degradation mechanism that impairs the safety and fast charge capabilities of automotive lithium-ion batteries. In this study, we present comprehensive investigation employing operando high-resolution optical microscopy combined with non-equilibrium thermodynamics implemented in a multi-dimensional (1D+1D to 3D) phase-field modeling framework to reveal the rate-dependent spatial dynamics of phase separation and plating in graphite electrodes. Here we visualize and provide mechanistic understanding of the multistage phase separation, plating, inter/intra-particle lithium exchange and plated lithium back-intercalation phenomena. A strong dependence of intra-particle lithiation heterogeneity on the particle size, shape, orientation, surface condition and C-rate at the particle level is observed, which leads to early onset of plating spatially resolved by a 3D image-based phase-field model. Moreover, we highlight the distinct relaxation processes at different state-of-charges (SOCs), wherein thermodynamically unstable graphite particles undergo a drastic intra-particle lithium redistribution and inter-particle lithium exchange at intermediate SOCs, whereas the electrode equilibrates much slower at low and high SOCs. These physics-based insights into the distinct SOC-dependent relaxation efficiency provide new perspective towards developing advanced fast charge protocols to suppress plating and shorten the constant voltage regime.
MIT Department
Massachusetts Institute of Technology. Department of Chemical Engineering
Massachusetts Institute of Technology. Department of Mathematics
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DOI of Published Version
https://doi.org/10.1038/s41467-023-40574-6
