Multiscale dynamics of charging and plating in graphite electrodes coupling operando microscopy and phase-field modelling

Lu, Xuekun; Lagnoni, Marco; Bertei, Antonio; Das, Supratim; Owen, Rhodri E.; Li, Qi; O’Regan, Kieran; Wade, Aaron; Finegan, Donal P.; Kendrick, Emma; Bazant, Martin Z.; Brett, Dan L.; Shearing, Paul R.

doi:10.1038/s41467-023-40574-6

Multiscale dynamics of charging and plating in graphite electrodes coupling operando microscopy and phase-field modelling

Journal Article · Thu Aug 24 04:00:00 EDT 2023 · Nature Communications

DOI:https://doi.org/10.1038/s41467-023-40574-6· OSTI ID:2005600

; ; ; ; Owen, Rhodri E.; ; ; ; ; ; ; ;

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.

View Accepted Manuscript (DOE)

Research Organization:: National Renewable Energy Laboratory (NREL), Golden, CO (United States)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE), Transportation Office. Vehicle Technologies Office

Grant/Contract Number:: AC36-08GO28308

OSTI ID:: 2005600

Alternate ID(s):: OSTI ID: 1999664

Report Number(s):: NREL/JA--5700-82021; MainId:82794; UUID:3ed7aafb-dac8-44bb-9000-45b88f7ac735; MainAdminID:70761

Journal Information:: Nature Communications, Journal Name: Nature Communications Journal Issue: 1 Vol. 14; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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Multiscale dynamics of charging and plating in graphite electrodes coupling operando microscopy and phase-field modelling

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