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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 ( IF 14.4 ) Pub Date : 2017-10-13 , DOI: 10.1021/jacs.7b06834 Yanting Jin 1 , Nis-Julian H. Kneusels 1 , Pieter C. M. M. Magusin 1 , Gunwoo Kim 1, 2 , Elizabeth Castillo-Martínez 1 , Lauren E. Marbella 1 , Rachel N. Kerber 1 , Duncan J. Howe 1 , Subhradip Paul 3 , Tao Liu 1 , Clare P. Grey 1
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2017-10-13 , DOI: 10.1021/jacs.7b06834 Yanting Jin 1 , Nis-Julian H. Kneusels 1 , Pieter C. M. M. Magusin 1 , Gunwoo Kim 1, 2 , Elizabeth Castillo-Martínez 1 , Lauren E. Marbella 1 , Rachel N. Kerber 1 , Duncan J. Howe 1 , Subhradip Paul 3 , Tao Liu 1 , Clare P. Grey 1
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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 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.
中文翻译：
确定使用添加剂氟代碳酸亚乙酯在硅上形成的固体电解质中间相稳定性提高的结构基础
为了阐明氟代碳酸亚乙酯（FEC）作为锂离子电池标准碳酸盐基电解质中添加剂的作用，在硅阳极电化学循环过程中形成的固体电解质界面（SEI）用溶液和固体的组合进行了分析。状态核磁共振技术，包括动态核极化。为了便于通过 1D 和 2D NMR 进行表征，我们合成了富含 13C 的 FEC，最终实现了有机 SEI 的详细结构分配。我们发现，在标准碳酸亚乙酯基电解质中循环后观察到的可溶性聚（环氧乙烷）类线性低聚电解质分解产物在 10 vol% FEC 添加剂存在下被抑制。FEC首先脱氟形成可溶性碳酸亚乙烯酯和乙烯基类物质，它们反应形成可溶性和不溶性支链环氧乙烷基聚合物。在不存在 FEC 的情况下，没有观察到支化聚合物的证据。
更新日期：2017-10-13
中文翻译：
确定使用添加剂氟代碳酸亚乙酯在硅上形成的固体电解质中间相稳定性提高的结构基础
为了阐明氟代碳酸亚乙酯（FEC）作为锂离子电池标准碳酸盐基电解质中添加剂的作用，在硅阳极电化学循环过程中形成的固体电解质界面（SEI）用溶液和固体的组合进行了分析。状态核磁共振技术，包括动态核极化。为了便于通过 1D 和 2D NMR 进行表征，我们合成了富含 13C 的 FEC，最终实现了有机 SEI 的详细结构分配。我们发现，在标准碳酸亚乙酯基电解质中循环后观察到的可溶性聚（环氧乙烷）类线性低聚电解质分解产物在 10 vol% FEC 添加剂存在下被抑制。FEC首先脱氟形成可溶性碳酸亚乙烯酯和乙烯基类物质，它们反应形成可溶性和不溶性支链环氧乙烷基聚合物。在不存在 FEC 的情况下，没有观察到支化聚合物的证据。
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