Multiscale Dynamics of Charging and Plating in Graphite Electrodes Coupling Operando Microscopy and Phase-Field Modelling

Xuekun Lu, Marco Lagnoni, Antonio Bertei, Supratim Das, Rhodri Owen, Qi Li, Kieran O'Regan, Aaron Wade, Donal Finegan, Emma Kendrick, Martin Bazant, Dan Brett, Paul Shearing

Research output: Contribution to journalArticlepeer-review

20 Scopus Citations

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.

Original languageAmerican English
Article numberArticle No. 5127
Number of pages14
JournalNature Communications
Volume14
Issue number1
DOIs
StatePublished - Dec 2023

Bibliographical note

Publisher Copyright:
© 2023, Springer Nature Limited.

NREL Publication Number

  • NREL/JA-5700-82021

Keywords

  • fast charging
  • Li plating
  • Li-ion batteries
  • modelling
  • operando imaging

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