Reduction Mechanism of Fluoroethylene Carbonate for Stable Solid–Electrolyte Interphase Film on Silicon Anode

Authors

  • Xilin Chen,

    1. Energy and Environment Directorate, Pacific Northwest National Laboratory, 902 Battelle Blvd., Richland, Washington 99352 (USA), Fax: (+1) 509/375-2186
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  • Xiaolin Li,

    1. Energy and Environment Directorate, Pacific Northwest National Laboratory, 902 Battelle Blvd., Richland, Washington 99352 (USA), Fax: (+1) 509/375-2186
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  • Donghai Mei,

    1. Fundamental and Computational Sciences Directorate, Pacific Northwest National Laboratory, 902 Battelle Blvd., Richland, Washington 99352 (USA)
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  • Ju Feng,

    1. Environmental and Molecular Sciences Laboratory, Pacific Northwest National Laboratory, 902 Battelle Blvd., Richland, Washington 99352 (USA)
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  • Mary Y. Hu,

    1. Fundamental and Computational Sciences Directorate, Pacific Northwest National Laboratory, 902 Battelle Blvd., Richland, Washington 99352 (USA)
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  • Jianzhi Hu,

    1. Fundamental and Computational Sciences Directorate, Pacific Northwest National Laboratory, 902 Battelle Blvd., Richland, Washington 99352 (USA)
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  • Mark Engelhard,

    1. Environmental and Molecular Sciences Laboratory, Pacific Northwest National Laboratory, 902 Battelle Blvd., Richland, Washington 99352 (USA)
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  • Jianming Zheng,

    1. Energy and Environment Directorate, Pacific Northwest National Laboratory, 902 Battelle Blvd., Richland, Washington 99352 (USA), Fax: (+1) 509/375-2186
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  • Wu Xu,

    1. Energy and Environment Directorate, Pacific Northwest National Laboratory, 902 Battelle Blvd., Richland, Washington 99352 (USA), Fax: (+1) 509/375-2186
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  • Jie Xiao,

    1. Energy and Environment Directorate, Pacific Northwest National Laboratory, 902 Battelle Blvd., Richland, Washington 99352 (USA), Fax: (+1) 509/375-2186
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  • Jun Liu,

    Corresponding author
    1. Energy and Environment Directorate, Pacific Northwest National Laboratory, 902 Battelle Blvd., Richland, Washington 99352 (USA), Fax: (+1) 509/375-2186
    • Energy and Environment Directorate, Pacific Northwest National Laboratory, 902 Battelle Blvd., Richland, Washington 99352 (USA), Fax: (+1) 509/375-2186

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  • Ji-Guang Zhang

    Corresponding author
    1. Energy and Environment Directorate, Pacific Northwest National Laboratory, 902 Battelle Blvd., Richland, Washington 99352 (USA), Fax: (+1) 509/375-2186
    • Energy and Environment Directorate, Pacific Northwest National Laboratory, 902 Battelle Blvd., Richland, Washington 99352 (USA), Fax: (+1) 509/375-2186

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Abstract

Fluoroethylene carbonate (FEC) is an effective electrolyte additive that can significantly improve the cycling ability of silicon and other anode materials. However, the fundamental mechanism of this improvement is still not well understood. Based on the results obtained from 6Li NMR and X-ray photoelectron spectroscopy studies, we propose a molecular-level mechanism for how FEC affects the formation of solid electrolyte interphase (SEI) film: 1) FEC is reduced through the opening of the five-membered ring leading to the formation of lithium poly(vinyl carbonate), LiF, and some dimers; 2) the FEC-derived lithium poly(vinyl carbonate) enhances the stability of the SEI film. The proposed reduction mechanism opens a new path to explore new electrolyte additives that can improve the cycling stability of silicon-based electrodes.

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