The application of rechargeable lithium metal batteries (LMBs) has been hindered by the fast growth of lithium dendrites during charge and the limited cycling life because of the decomposition of the electrolyte at the interface. Here, we have developed a non-flammable triethyl phosphate (TEP)-based electrolyte with tris(hexafluoroisopropyl)phosphate (THFP) as an additive. The polar nature of the C-F bonding and the rich CF3 groups in THFP lowers its LUMO energy and HOMO energy to help form a stable, LiF-rich solid electrolyte interphase (SEI) layer through the reduction of THFP and increases the binding ability of the PF6- anions, which significantly suppresses lithium dendrite growth and reduces the electrolyte decomposition. Moreover, THFP participates in the formation of a thin, C-F rich electrolyte interphase (CEI) layer to provide the stable cycling of the cathode at a high voltage. The symmetric Li||Li and full Li/NCM622 cells with THFP additive have small polarization and long cycling life, which demonstrates the importance of the additive to the application of the LMBs.
Keywords: Electrolytes; Lithium dendrites; Lithium metal batteries; Non-flammable electrolytes; Solid state interphase.
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