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Regulating interfacial stability of SiOx anode with fluoride-abundant solid–electrolyte interphase by fluorine-functionalized additive

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Abstract

Silicon oxide (SiOx) has received remarkable attention as a next-generation battery material; however, the sudden decrease in the cycling retention constitutes a significant challenge in facilitating its application. Tris(2,2,2-trifluoroethyl) phosphite (TTFP), which can control parasitic reactions such as the pulverization of SiOx anode materials and electrolyte decomposition, has been proposed to improve the lifespan of the cell. The electrochemical reduction of TTFP results in solid-electrolyte interphase (SEI) layers that are mainly composed of LiF, which occur at a higher potential than the working potential of the SiOx anode and carbonate-based solvents. The electrolyte with TTFP exhibited a substantial improvement in cycling retention after 100 cycles, whereas the standard electrolyte showed acutely decreased retention. The thickness of the SiOx anode with TTFP also changed only slightly without any considerable delamination spots, whereas the SiOx anode without TTFP was prominently deformed by an enormous volume expansion with several internal cracks. The cycled SiOx anode with TTFP exhibited less increase in resistance after cycling than that in the absence of TTFP, in addition to fewer decomposition adducts in corresponding X-ray photoelectron spectroscopy (XPS) analyses between the cycled SiOx anodes. These results demonstrate that TTFP formed SEI layers at the SiOx interface, which substantially reduced the pulverization of the SiOx anode materials; in addition, electrolyte decomposition at the interface decreased, which led to improved cycling retention.

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Acknowledgements

This work was financially supported by the National Research Foundation of Korea financially (NRF) (No. NRF-2022R1F1A1069039), the Core Research Institute (CRI) Program, the Basic Science Research Program through the National Research Foundation of Korea (NRF), Ministry of Education (No. NRF-2017R1A6A1A06015181) and the Technology Innovation Program (No. 20011905) funded by the Ministry of Trade, Industry & Energy (MOTIE, Korea). We are also thanks to Kyeongsuk Park (Applied Spectra, Inc.) for the assistance of LIBS measurements.

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  1. Advanced Batteries Laboratory, Department of Chemistry, Incheon National University, Incheon, 22012, Republic of Korea

    Subin Lee & Taeeun Yim

  2. Research Institute of Basic Sciences, College of Natural Science, Incheon National University, Incheon, 22012, Republic of Korea

    Subin Lee & Taeeun Yim

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Lee, S., Yim, T. Regulating interfacial stability of SiOx anode with fluoride-abundant solid–electrolyte interphase by fluorine-functionalized additive. Rare Met. 43, 671–681 (2024). https://doi.org/10.1007/s12598-023-02474-y

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  • DOI: https://doi.org/10.1007/s12598-023-02474-y

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