Rechargeable Li-metal batteries using high-voltage cathodes can deliver the highest possible energy densities among all electrochemistries. However, the notorious reactivity of metallic lithium as well as the catalytic nature of high-voltage cathode materials largely prevents their practical application. Here, we report a non-flammable fluorinated electrolyte that supports the most aggressive and high-voltage cathodes in a Li-metal battery. Our battery shows high cycling stability, as evidenced by the efficiencies for Li-metal plating/stripping (99.2%) for a 5 V cathode LiCoPO (~99.81%) and a Ni-rich LiNiMnCoO cathode (~99.93%). At a loading of 2.0 mAh cm, our full cells retain ~93% of their original capacities after 1,000 cycles. Surface analyses and quantum chemistry calculations show that stabilization of these aggressive chemistries at extreme potentials is due to the formation of a several-nanometre-thick fluorinated interphase.

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Li metal is regarded as the ''Holy Grail'' electrode because of its highest specific capacity and lowest electrochemical potential. However, challenges arising from the low Coulombic efficiency (CE) and dendritic nature of Li metal in carbonate electrolytes remain to be resolved. Here, by increasing LiFSI salt concentration in the carbonate electrolyte, we successfully increased the CE to 99.3% while suppressing Li dendrite formation. An NMC622jjLi cell was paired and showed excellent cycling performance.

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