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  5. Lithium-metal batteries (LMBs) are promising alternatives to state-of-the-art Lithium-ion batteries (LIBs) to achieve higher energy densities. However, the poor cyclability of LMBs resulting from Li metal anode (Li0) irreversibility and concomitant electrolyte decompositions limits their practical applications. In this study, we reported a per-fluorinated salt, lithium tetrakis(perfluoro-tertbutyloxy)borate (abbreviated as Li-TFOB) as an electrolyte additive for Li-metal batteries, which contains 36 F atoms per molecule. This newly designed ionic additive tuned the chemical composition of the solid-electrolyte interphase (SEI) on Li0 by increasing the amount of LiF and Li-B-O inorganic species. DFT calculations and Molecular dynamics (MD) simulations indicated the preferential reduction of the TFOB anions at Li0, which occurs with a lower free energy change than PF6anions. The designed ionic additive enables the 4.6 V Li||LiNi0.6Mn0.2Co0.2O2 (NMC622) cell to achieve an average CE of 99.1 % and a high-capacity retention of >50 % after 500 cycles. This experiment-simulation joint study illustrated an attractive approach to accelerating the design of electrolytes and interphases for LMBs. 
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