Identifying the structural basis for the increased stability of the solid electrolyte interphase formed on silicon with the additive fluoroethylene carbonate

Identifying the structural basis for the increased stability of the solid electrolyte interphase formed on silicon with the additive fluoroethylene carbonate. Jin, Y., Kneusels, N., Magusin, P., Kim, G., Castillo-Martínez, E., Marbella, L., Kerber, R., Howe, D., Paul, S., Liu, T., & Grey, C. 2018. Publication Title: arXiv
abstract bibtex

Copyright © 2018, arXiv, All rights reserved. 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 13C-enriched FEC, ultimately allowing a detailed structural assignment of the organic SEI. We find that the soluble PEO-like linear oligomeric electrolyte breakdown products that are observed after cycling in the standard ethylene carbonate (EC)-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 are observed in the absence of FEC.

@misc{jin_identifying_2018,
	title = {Identifying the structural basis for the increased stability of the solid electrolyte interphase formed on silicon with the additive fluoroethylene carbonate},
	abstract = {Copyright © 2018, arXiv, All rights reserved. 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 13C-enriched FEC, ultimately allowing a detailed structural assignment of the organic SEI. We find that the soluble PEO-like linear oligomeric electrolyte breakdown products that are observed after cycling in the standard ethylene carbonate (EC)-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 are observed in the absence of FEC.},
	author = {Jin, Y. and Kneusels, N.-J.H. and Magusin, P.C.M.M. and Kim, G. and Castillo-Martínez, E. and Marbella, L.E. and Kerber, R.N. and Howe, D.J. and Paul, S. and Liu, T. and Grey, C.P.},
	year = {2018},
	note = {Publication Title: arXiv},
	keywords = {\#nosource},
}

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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 13C-enriched FEC, ultimately allowing a detailed structural assignment of the organic SEI. We find that the soluble PEO-like linear oligomeric electrolyte breakdown products that are observed after cycling in the standard ethylene carbonate (EC)-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. 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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 13C-enriched FEC, ultimately allowing a detailed structural assignment of the organic SEI. We find that the soluble PEO-like linear oligomeric electrolyte breakdown products that are observed after cycling in the standard ethylene carbonate (EC)-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. 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