On the dynamics of the fluoroethylene carbonate generated solid electrolyte interphase on silicon anodes during calendar life aging

Barua, Sattajit; Abraham, Daniel P.; Yao, Koffi Pierre Claver

doi:10.1016/j.electacta.2025.146624

On the dynamics of the fluoroethylene carbonate generated solid electrolyte interphase on silicon anodes during calendar life aging

Journal Article · Wed Jun 04 00:00:00 EDT 2025 · Electrochimica Acta

DOI:https://doi.org/10.1016/j.electacta.2025.146624· OSTI ID:3021817

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Univ. of Delaware, Newark, DE (United States)
Argonne National Laboratory (ANL), Argonne, IL (United States)

Here, the widespread use of silicon (Si)-rich anodes in lithium-ion batteries (LIBs) is impeded by an unstable solid electrolyte interphase (SEI) incurring insufficient cell life. Fluoroethylene carbonate (FEC) additive in the electrolyte significantly improves cycle life. However, the gains on calendar life remain unclear; the SEI structure still undergoes detrimental alterations at rest. Thus, elucidating the SEI dynamics during calendar aging is critical to mitigating time-dependent capacity degradation. ATR-FTIR, XPS, and ToF-SIMS are used herein to investigate the SEI structure before and after calendar aging. Si cycled without FEC exhibits no notable SEI chemistry changes Pre- and Post-aging, leaving poor passivation as the main failure pathway. Conversely, the FEC-SEI starts as short oligomeric species from FEC/EC electroreduction prior to aging; after calendar aging, polymerized carbonates become consistently more prominent. Unexpectedly, the deposition of self-polymerized FEC species results from time exposure to the delithiated Si specifically as opposed to the lithiated surface. This unexpected finding is supported by another recent Si calendar-aging research, which albeit not investigating FEC, finds global failure of the SEI upon delithiation resulting in ∼247 fold more reactive surface compared to the lithiated.

View Accepted Manuscript (DOE)

Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: National Science Foundation (NSF); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Office of Sustainable Transportation. Vehicle Technologies Office (VTO)

Grant/Contract Number:: AC02-06CH11357; EE0009185

Other Award/Contract Number:: DMR-2116754
1428149

OSTI ID:: 3021817

Journal Information:: Electrochimica Acta, Journal Name: Electrochimica Acta Vol. 535; ISSN 0013-4686

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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On the dynamics of the fluoroethylene carbonate generated solid electrolyte interphase on silicon anodes during calendar life aging

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