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Chemo-Mechanical Model of SEI Growth on Silicon Electrode Particles**

von Kolzenberg, Lars and Latz, Arnulf and Horstmann, Birger (2021) Chemo-Mechanical Model of SEI Growth on Silicon Electrode Particles**. Batteries & Supercaps, n/a (n/a). Wiley. doi: 10.1002/batt.202100216. ISSN 2566-6223.

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Official URL: https://chemistry-europe.onlinelibrary.wiley.com/doi/abs/10.1002/batt.202100216

Abstract

Abstract Silicon anodes promise high energy densities of next-generation lithium-ion batteries, but suffer from shorter cycle life. The accelerated capacity fade stems from the repeated fracture and healing of the solid-electrolyte interphase (SEI) on the silicon surface. This interplay of chemical and mechanical effects in SEI on silicon electrodes causes a complex aging behavior. However, so far, no model mechanistically captures the interrelation between mechanical SEI deterioration and accelerated SEI growth. In this article, we present a thermodynamically consistent continuum model of an electrode particle surrounded by an SEI layer. The silicon particle model consistently couples chemical reactions, physical transport, and elastic deformation. The SEI model comprises elastic and plastic deformation, fracture, and growth. Capacity fade measurements on graphite anodes and in-situ mechanical SEI measurements on lithium thin films provide parametrization for our model. For the first time, we model the influence of cycling rate on the long-term mechanical SEI deterioration and regrowth. Our model predicts the experimentally observed transition in time dependence from square-root-of-time growth during battery storage to linear-in-time growth during continued cycling. Thereby our model unravels the mechanistic dependence of battery aging on operating conditions and supports the efforts to prolong the battery life of next-generation lithium-ion batteries.

Item URL in elib:https://elib.dlr.de/147458/
Document Type:Article
Title:Chemo-Mechanical Model of SEI Growth on Silicon Electrode Particles**
Authors:
AuthorsInstitution or Email of AuthorsAuthor's ORCID iD
von Kolzenberg, LarsLars.Kolzenberg (at) dlr.deUNSPECIFIED
Latz, ArnulfArnulf.Latz (at) dlr.deUNSPECIFIED
Horstmann, Birgerbirger.horstmann (at) dlr.deUNSPECIFIED
Date:2021
Journal or Publication Title:Batteries & Supercaps
Refereed publication:Yes
Open Access:No
Gold Open Access:No
In SCOPUS:Yes
In ISI Web of Science:Yes
Volume:n/a
DOI :10.1002/batt.202100216
Publisher:Wiley
ISSN:2566-6223
Status:Published
Keywords:continuum modeling, lithium-ion batteries, mechanical properties, solid-electrolyte interphase (SEI), thermodynamics
HGF - Research field:Energy
HGF - Program:Materials and Technologies for the Energy Transition
HGF - Program Themes:Electrochemical Energy Storage
DLR - Research area:Energy
DLR - Program:E SP - Energy Storage
DLR - Research theme (Project):E - Electrochemical Storage
Location: Ulm
Institutes and Institutions:Institute of Engineering Thermodynamics > Computational Electrochemistry
Deposited By: Horstmann, Birger
Deposited On:23 Dec 2021 21:04
Last Modified:23 Dec 2021 21:04

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