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

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 opera...

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Autores principales: 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 J. L., Shearing, Paul R.
Formato: Online Artículo Texto
Lenguaje:English
Publicado: Nature Publishing Group UK 2023
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10449918/
https://www.ncbi.nlm.nih.gov/pubmed/37620348
http://dx.doi.org/10.1038/s41467-023-40574-6
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author 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 J. L.
Shearing, Paul R.
author_facet 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 J. L.
Shearing, Paul R.
author_sort Lu, Xuekun
collection PubMed
description 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.
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spelling pubmed-104499182023-08-26 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 J. L. Shearing, Paul R. Nat Commun Article 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. Nature Publishing Group UK 2023-08-24 /pmc/articles/PMC10449918/ /pubmed/37620348 http://dx.doi.org/10.1038/s41467-023-40574-6 Text en © The Author(s) 2023 https://creativecommons.org/licenses/by/4.0/Open Access This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons license and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/ (https://creativecommons.org/licenses/by/4.0/) .
spellingShingle Article
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 J. L.
Shearing, Paul R.
Multiscale dynamics of charging and plating in graphite electrodes coupling operando microscopy and phase-field modelling
title Multiscale dynamics of charging and plating in graphite electrodes coupling operando microscopy and phase-field modelling
title_full Multiscale dynamics of charging and plating in graphite electrodes coupling operando microscopy and phase-field modelling
title_fullStr Multiscale dynamics of charging and plating in graphite electrodes coupling operando microscopy and phase-field modelling
title_full_unstemmed Multiscale dynamics of charging and plating in graphite electrodes coupling operando microscopy and phase-field modelling
title_short Multiscale dynamics of charging and plating in graphite electrodes coupling operando microscopy and phase-field modelling
title_sort multiscale dynamics of charging and plating in graphite electrodes coupling operando microscopy and phase-field modelling
topic Article
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10449918/
https://www.ncbi.nlm.nih.gov/pubmed/37620348
http://dx.doi.org/10.1038/s41467-023-40574-6
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