Unraveling Morphology and Chemistry Dynamics in Fluoroethylene Carbonate Generated Silicon Anode Solid Electrolyte Interphase Across Delithiated and Lithiated States: Relative Cycling Stability Enabled by an Elastomeric Polymer Matrix

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Author(s)Mou, Rownak J.
Author(s)Barua, Sattajit
Author(s)Abraham, Daniel P.
Author(s)Yao, Koffi P. C.
Date Accessioned2024-04-30T19:34:50Z
Date Available2024-04-30T19:34:50Z
Publication Date2024-04-25
DescriptionThis article was originally published in Journal of The Electrochemical Society. The version of record is available at: https://doi.org/10.1149/1945-7111/ad3ec4. © 2024 The Author(s). Published on behalf of The Electrochemical Society by IOP Publishing Limited. This is an open access article distributed under the terms of the Creative Commons Attribution Non-Commercial No Derivatives 4.0 License (CC BY NC-ND, http://creativecommons.org/licenses/by-nc-nd/4.0/), which permits non-commercial reuse, distribution, and reproduction in any medium, provided the original work is not changed in any way and is properly cited. For permission for commercial reuse, please email: permissions@ioppublishing.org. [DOI: 10.1149/1945-7111/ad3ec4]
AbstractThe silicon solid electrolyte interphase (SEI) faces cyclical cracking and reconstruction due to the ∼350% volume expansion. Understanding the SEI dynamic morphology and chemistry evolution from delithiated to lithiated states is thereby paramount to engineering a stable Si anode. Fluoroethylene carbonate (FEC) is a preferred additive with widely demonstrated enhancement of the Si cycling. Thus, insights into the dynamics of the FEC-SEI may provide hints toward engineering the Si interface. Herein, complementary ATR-FTIR, AFM, tip IR, and XPS probing reveal the presence of an elastomeric polycarbonate-like matrix in the FEC-generated SEI which is absent from the FEC-free SEI. Adding FEC to the baseline 1 M LiPF6 in EC:EMC (1:1) electrolyte promotes formation of a thinner and more conformal SEI, and subdues morphology and chemistry changes between consecutive half-cycles. From AFM, morphological stabilization of the FEC-SEI occurs earlier. Furthermore, conventional SEI biproducts such as Li2CO3 and LiEDC appear in reduced quantities in the FEC-SEI implying a reduced quantity of Li-consuming species. The thin polymeric FEC-SEI enables deeper (de)lithiation of silicon. In conclusion, the enhanced mechanical compliance, chemical invariance, and reduced Li inventory consumption of the FEC-SEI are logically the key features underlying the Si cycling enhancement by FEC.
SponsorThis work is funded by the U.S. Department of Energy's Office of Energy Efficiency and Renewable Energy (EERE) under the Award Number DE-EE0009185. The authors would like to acknowledge the assistance of Gerald Poirier and Jing Qu from the Advance Materials Characterization Laboratory (AMCL) at University of Delaware with AFM-NanoIR and ATR-FTIR techniques. We also acknowledge the Surface Analysis Facility (SAF) at University of Delaware for giving access to Thermo Scientific K-Alpha XPS system (NSF award No. 1428149).
CitationMou, Rownak J., Sattajit Barua, Daniel P. Abraham, and Koffi P. C. Yao. “Unraveling Morphology and Chemistry Dynamics in Fluoroethylene Carbonate Generated Silicon Anode Solid Electrolyte Interphase Across Delithiated and Lithiated States: Relative Cycling Stability Enabled by an Elastomeric Polymer Matrix.” Journal of The Electrochemical Society 171, no. 4 (2024): 040546. https://doi.org/10.1149/1945-7111/ad3ec4.
ISSN1945-7111
URLhttps://udspace.udel.edu/handle/19716/34330
Languageen_US
PublisherJournal of The Electrochemical Society
dc.rightsAttribution-NonCommercial-NoDerivatives 4.0 Internationalen
dc.rights.urihttp://creativecommons.org/licenses/by-nc-nd/4.0/
TitleUnraveling Morphology and Chemistry Dynamics in Fluoroethylene Carbonate Generated Silicon Anode Solid Electrolyte Interphase Across Delithiated and Lithiated States: Relative Cycling Stability Enabled by an Elastomeric Polymer Matrix
TypeArticle
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