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 E. Owen, Qi Li, Kieran O’Regan, Aaron Wade, Donal P. Finegan, Emma Kendrick, Martin Z. Bazant, Dan J. L. Brett and Paul R. Shearing ()
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Xuekun Lu: Department of Chemical Engineering, UCL
Marco Lagnoni: University of Pisa
Antonio Bertei: University of Pisa
Supratim Das: MIT
Rhodri E. Owen: Department of Chemical Engineering, UCL
Qi Li: Beijing University of Technology
Kieran O’Regan: Harwell Science and Innovation Campus
Aaron Wade: Department of Chemical Engineering, UCL
Donal P. Finegan: National Renewable Energy Laboratory
Emma Kendrick: Harwell Science and Innovation Campus
Martin Z. Bazant: MIT
Dan J. L. Brett: Department of Chemical Engineering, UCL
Paul R. Shearing: Department of Chemical Engineering, UCL

Nature Communications, 2023, vol. 14, issue 1, 1-14

Abstract: 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.

Date: 2023
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DOI: 10.1038/s41467-023-40574-6

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