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Stabilized High-Voltage Cathodes via an F‑Rich and Si-Containing Electrolyte Additive
journal contribution
posted on 2020-06-09, 18:05 authored by Yuanqin Li, Kang Wang, Jiawei Chen, Wenguang Zhang, Xuehuan Luo, Zhangmin Hu, Qiankui Zhang, Lidan Xing, Weishan LiHigh-voltage
cathodes provide a promising solution to the energy
density limitation of currently commercialized lithium-ion batteries,
but they are unstable in electrolytes during the charge/discharge
process. To address this issue, we propose a novel electrolyte additive,
pentafluorophenyltriethoxysilane (TPS), which is rich in elemental
F and contains elemental Si. The effectiveness of TPS has been demonstrated
by cycling a representative high-voltage cathode, LiNi0.5Mn1.5O4 (LNMO), in 1.0 M LiPF6–diethyl
carbonate/ethylene carbonate/ethyl methyl carbonate (2/3/5 in weight).
LNMO presents an increased capacity retention from 28 to 85% after
400 cycles at 1 C by applying 1 wt % TPS. Further electrochemical
measurements combined with spectroscopic characterization and theoretical
calculations indicate that TPS can not only construct a robust protective
cathode electrolyte interphase via its oxidation during initial lithium
desertion but also scavenge the detrimental hydrogen fluoride (HF)
present in the electrolyte via its strong combination with the species
HF, F–, and H+, highly stabilizing LNMO
during the charge/discharge process. These features of TPS provide
a new solution to the obstacle in the practical application of high-voltage
cathodes not limited to LNMO.
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Keywords
LNMOchargehydrogen fluorideTPSsolutionLiNi 0.5 Mn 1.5 O 4energy density limitationcathode electrolyte interphasespectroscopic characterizationStabilized High-Voltage Cathodeslithium desertioncarbonatecapacity retentionspecies HF1 Cnovel electrolyte additiveelectrochemical measurements400 cycleslithium-ion batteriesSi-Containing Electrolyte Additive High-voltage cathodes
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