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Identifying the Mechanism of Continued Growth of the Solid-Electrolyte Interphase

Single, Fabian and Latz, Arnulf and Horstmann, Birger (2018) Identifying the Mechanism of Continued Growth of the Solid-Electrolyte Interphase. ChemSusChem, 11 (12), pp. 1950-1955. Wiley. doi: 10.1002/cssc.201800077. ISSN 1864-5631.

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Official URL: https://onlinelibrary.wiley.com/doi/abs/10.1002/cssc.201800077


Continued growth of the solid-electrolyte interphase (SEI) is the major reason for capacity fade in modern lithium-ion batteries. This growth is made possible by a yet unidentified transport mechanism that limits the passivating ability of the SEI towards electrolyte reduction. We, for the first time, differentiate the proposed mechanisms by analyzing their dependence on the electrode potential. Our calculations are compared to recent experimental capacity-fade data. We show that the potential dependence of SEI growth facilitated by solvent diffusion, electron conduction, or electron tunneling qualitatively disagrees with the experimental observations. Only diffusion of Li interstitials results in a potential dependence matching the experiments. Therefore, we identify the diffusion of neutral radicals, such as Li interstitials, as the cause of long‐term SEI growth.

Item URL in elib:https://elib.dlr.de/124806/
Document Type:Article
Title:Identifying the Mechanism of Continued Growth of the Solid-Electrolyte Interphase
AuthorsInstitution or Email of AuthorsAuthor's ORCID iD
Single, Fabianfabian.single (at) dlr.dehttps://orcid.org/0000-0003-1658-5077
Latz, Arnulfarnulf.latz (at) dlr.dehttps://orcid.org/0000-0003-1449-8172
Horstmann, Birgerbirger.horstmann (at) dlr.dehttps://orcid.org/0000-0002-1500-0578
Date:12 March 2018
Journal or Publication Title:ChemSusChem
Refereed publication:Yes
Open Access:Yes
Gold Open Access:No
In ISI Web of Science:Yes
DOI :10.1002/cssc.201800077
Page Range:pp. 1950-1955
Series Name:Interfacing Theory and Experiment
Keywords:SEI, Lithium-Ion, Battery Degradation
HGF - Research field:Energy
HGF - Program:Storage and Cross-linked Infrastructures
HGF - Program Themes:Electrochemical Energy Storage
DLR - Research area:Energy
DLR - Program:E SP - Energy Storage
DLR - Research theme (Project):E - Electrochemical Prcesses (Batteries) (old)
Location: Braunschweig
Institutes and Institutions:Institute of Engineering Thermodynamics > Computational Electrochemistry
Deposited By: Single, Fabian
Deposited On:20 Dec 2018 14:34
Last Modified:31 Jul 2019 20:22

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