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Cited by 946Advanced Battery Technologies ResearchAdvancements in Battery MaterialsAdvanced Battery Materials and Technologies

Theory of SEI formation in rechargeable batteries: capacity fade, accelerated aging and lifetime prediction

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Pinson, Matthew B., Bazant, Martin Z.·2013·Journal of The Electrochemical Society
DOI 10.1149/2.044302jes
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Abstract

Cycle life is critically important in applications of rechargeable batteries, but lifetime prediction is mostly based on empirical trends, rather than mathematical models. In practical lithium-ion batteries, capacity fade occurs over thousands of cycles, limited by slow electrochemical processes, such as the formation of a solid-electrolyte interphase (SEI) in the negative electrode, which compete with reversible lithium intercalation. Focusing on SEI growth as the canonical degradation mechanism, we show that a simple single-particle model can accurately explain experimentally observed capacity fade in commercial cells with graphite anodes, and predict future fade based on limited accelerated aging data for short times and elevated temperatures. The theory is extended to porous electrodes, predicting that SEI growth is essentially homogeneous throughout the electrode, even at high rates. The lifetime distribution for a sample of batteries is found to be consistent with Gaussian statistics, as predicted by the single-particle model. We also extend the theory to rapidly degrading anodes, such as nanostructured silicon, which exhibit large expansion on ion intercalation. In such cases, large area changes during cycling promote SEI loss and faster SEI growth. Our simple models are able to accurately fit a variety of published experimental data for graphite and silicon anodes.

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  • Most physics-based models focus only on the most dominant degradation mechanisms, such as SEI formation and growth or electronic contact loss through particle cracking.

    “which is why most physics-based models focus only on the most dominant mechanisms, such as the formation and growth of the solid electrolyte interphase (SEI) [11,12] or electronic contact loss through particle cracking [13,14].”

    From Degradation diagnostics for lithium ion cells (2017) · cites this paper as [11]

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Authors
Pinson, M. B., & Bazant, M. Z.
Affiliations
Massachusetts Institute of Technology (US)
ORCID
Venue
Journal of The Electrochemical Society
Publisher
The Electrochemical Society
Published
2012-12-01
Volume
160
Issue
2
Pages
A243-A250
ISSN
  • 0013-4651 (ISSN-L)
  • 1945-7111
DOI
10.1149/2.044302jes
OpenAlex
W2340971382
Cited by
946
References
53
Citations by year
2026: 83 · 2025: 74 · 2024: 79 · 2023: 79 · 2022: 82 · 2021: 91 · 2020: 75 · 2019: 85 · 2018: 76 · 2017: 77 · 2016: 53 · 2015: 50 · 2014: 32 · 2013: 10
FWCI
52.98
Type
journal article
Language
en
Open access
Locations
Journal of The Electrochemical Society (publishedVersion)
Funders
Samsung
Topics
  • Physical Sciences › Engineering › Automotive Engineering › Advanced Battery Technologies Research
  • Physical Sciences › Engineering › Electrical and Electronic Engineering › Advancements in Battery Materials
  • Physical Sciences › Engineering › Electrical and Electronic Engineering › Advanced Battery Materials and Technologies
Keywords
solid electrolyte interphase, lithium-ion batteries, capacity fade, accelerated aging, battery lifetime prediction, single particle model, graphite anode, porous electrodes, silicon anodes, electrode expansion, battery degradation mechanisms

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