CUED Publications database

Identifying the Structural Basis for the Increased Stability of the Solid Electrolyte Interphase Formed on Silicon with the Additive Fluoroethylene Carbonate

Jin, Y and Kneusels, NJH and Magusin, PCMM and Kim, G and Castillo-Martínez, E and Marbella, LE and Kerber, RN and Howe, DJ and Paul, S and Liu, T and Grey, CP (2017) Identifying the Structural Basis for the Increased Stability of the Solid Electrolyte Interphase Formed on Silicon with the Additive Fluoroethylene Carbonate. Journal of the American Chemical Society, 139. pp. 14992-15004. ISSN 0002-7863

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Abstract

To elucidate the role of fluoroethylene carbonate (FEC) as an additive in the standard carbonate-based electrolyte for Li-ion batteries, the solid electrolyte interphase (SEI) formed during electrochemical cycling on silicon anodes was analyzed with a combination of solution and solid-state NMR techniques, including dynamic nuclear polarization. To facilitate characterization via 1D and 2D NMR, we synthesized C-enriched FEC, ultimately allowing a detailed structural assignment of the organic SEI. We find that the soluble poly(ethylene oxide)-like linear oligomeric electrolyte breakdown products that are observed after cycling in the standard ethylene carbonate-based electrolyte are suppressed in the presence of 10 vol% FEC additive. FEC is first defluorinated to form soluble vinylene carbonate and vinoxyl species, which react to form both soluble and insoluble branched ethylene-oxide-based polymers. No evidence for branched polymers is observed in the absence of FEC. 13

Item Type: Article
Subjects: UNSPECIFIED
Divisions: Div B > Solid State Electronics and Nanoscale Science
Depositing User: Cron Job
Date Deposited: 22 Nov 2017 20:11
Last Modified: 15 Apr 2021 05:48
DOI: 10.1021/jacs.7b06834