High-Efficiency Lithium-Metal Anode Enabled by Liquefied Gas Electrolytes

Among the several challenges to enable next-generation batteries is the development of an electrolyte that maintains a dendrite-free and high Coulombic efficiency lithium-metal anode over extended cell cycling. A new electrolyte solvation structure and transport mechanism is demonstrated in fluoromethane-based liquefied gas electrolytes with the introduction of additive amounts of tetrahydrofuran, which is shown to fully coordinate with the lithium cations and greatly enhance salt dissociation and transport. The resulting electrolyte shows a high conductivity and transference number (t+ > 0.79), which leads to a dramatic improvement of the cycling performance of the lithium-metal anode. Systems using the enhanced liquefied gas electrolytes demonstrate a long-term high average Coulombic efficiency of 99.6%, 99.4%, and 98.1% (± 0.3%) at capacities of 0.5, 1, and 3 mAh·cm−2, respectively, with dendrite-free morphology and remarkable rate capability. Both the rate and cycling performance are well maintained from +20°C to −60°C.